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In June 2019, Tsui finished her Master's Degree in Psychology at the University of Hong Kong.

In 2015, Tsui's management contract with TVB ended. However, Tsui said that she is still on very good terms with TVB, and TVB has settled job arrangements for her up until February 2016. Despite having received several offers, Tsui stated that she will not finalize any management contract agreements until she has completed her jewelry design courses.

In 2015, Tsui was cast in thriller film, Knock Knock, Who's There?. The film is the first directorial effort by veteran actress, Carrie Ng. Tsui said that upon receiving the script, she had intended to reject the role because of the frightening content. However, Tsui eventually agreed to the role due to Ng's persistence and persuasion. With reference to collaborating with Tsui, Ng said that Tsui is a very professional and admirable actress.

In December 2015, Tsui launched a jewelry line with K.S. Sze & Sons Ltd.. The collection is called "Rabbit-Duck Illusion". She indicated that her designs are inspired by Ludwig Wittgenstein's concept on the two different ways of seeing, using the ambiguous image of a "duckrabbit". She spoke of the concept behind her jewelry designs, "It's something that I like to remind myself of, that there are many situations in life that aren't worth splitting hairs over, and if I simply adjust the angle that I'm viewing things from, I can easily see a different perspective." In early 2016, Tsui found her own fine jewelry brand and online shop; katetsui.com

In 2015-2016, Tsui completed her Jewelry Design course at GIA and Colored Gem Professional Level II at the Gübelin Academy.

In 2014, Tsui took part in a TVB-produced micro film, A Time of Love, which consists of four individual stories, each with a separate theme. Tsui starred opposite Taiwanese actors, James Wen and Chris Wang, in the "sorrow" themed story. After the airing of the micro film, TVB received 39 individual viewer statements that commended Tsui of her outstanding performance in the micro film. Column writer, Ko Leung, of Macao Daily, also stated Tsui portrayed her character in the micro film perfectly and that Tsui's acting is comparable to that of Bai Baihe in The Stolen Years.

In 2014, Tsui had originally been cast in the film version of Triumph in the Skies, starring opposite Louis Koo. However, for unspecified reasons, Tsui was eventually pulled out of the film and replaced with Charmaine Sheh.

Nominated — TVB Star Awards Malaysia 2014 for My Favourite TVB On-Screen Couple (Dayo Wong & Kate Tsui) (Top 3) Won — StarHub TVB Awards 2014 for My Top 6 Favourite TVB Female TV Character

Nominated — StarHub TVB Awards 2014 for My Favourite TVB On-Screen Couple (Bosco Wong & Kate Tsui) (Top 5)

With her performance in Eye in the Sky, Tsui earned the Best Newcomer – Gold Award from Hong Kong Film Directors' Guild 2007, as well as Hong Kong Film Award for Best New Performer from the 27th Hong Kong Film Awards, held in 2008. The latter is a particularly outstanding achievement, for Tsui is, so far, the only individual to have received a Hong Kong Film Award, while being fully contracted by TVB, since Anita Yuen, who coincidentally is also a Miss Hong Kong pageant winner, won the same award back in 1993.

In 2013, Tsui took part in a comedy film, I Love Hong Kong 2013. It is also the first film that veteran actress, Veronica Yip, has taken part in since her retirement in 1996. In the film, Tsui plays the younger version of Yip's character. The producer of the film, Eric Tsang, specifically praised Tsui for providing the best performance out of the entire cast, referring to it as a "Best Actress performance".

2012 is arguably Tsui's peak year in her TV career. In Highs and Lows, Tsui portrays an extremely tragic character that struggled with substance abuse, gang rape, and eventually, drug dealing. Tsui described her experience of filming this drama as "being on an emotional roller coaster", to the extent that she did not wish to speak to anyone or pick up the phone after work. The producer of the drama, Lam Chi Wah, referred to Tsui's role in Highs and Lows as the greatest breakthrough in her career and applauded her for setting down her image as a beauty pageant winner to dive into such a complex character in the drama. Film director, Patrick Kong, also noted in his column that Tsui's acting has greatly matured in Highs and Lows, particularly in her portrayal of emotional scenes.

The role at last earned her the Favourite Female Character award for the TVB Anniversary Awards 2012. Tsui was also nominated in the Best Actress category and was one of the top 5 finalists for the award. Aside from the aforementioned Hong Kong TVB-based awards show, Tsui also received a nomination for Best Actress in a Leading Role for the Asian Television Awards, which is an awards show held in Singapore that recognizes production excellence in over 15 Asian countries.

Additionally, in 2011, with the high turnover rate in contracted TVB artists, TVB executive, Virginia Lok, appointed Tsui, Myolie Wu, Linda Chung, and Fala Chen, as the new Top 4 "Fa Dans" (a Cantonese term that is used for actresses with high popularity and status in TVB), with their predecessors being Flora Chan, Ada Choi, Kenix Kwok, and Jessica Hsuan.

In 2011, Tsui reprised her role as Paris Yiu Ho Ho from the TVB series Lives of Omission in its film sequel, Turning Point 2, in which she starred opposite Francis Ng. Playing a character with a mental disorder in the film, Tsui said that collaborating with Ng was a valuable experience because Ng was extremely willing to teach and give her suggestions about her acting and performances. From working with Tsui, Ng had openly praised her for her acting potential.

In 2010, Tsui starred in Wuxia film 14 Blades, alongside Donnie Yen, Zhao Wei, and Wu Chun. The director of the film, Daniel Lee, said the casting of Tsui's character, Tuo Tuo, was the most troubling and extensive process of all. She eventually won the role while being backed by nearly half the votes of a public online poll held by Sina, in addition to being a Hong Kong Film Awards recipient.

While Tsui's TV career quieted down during 2009 to 2010, due to her focus on her film career, 2011 proved to be fruitful for Tsui, with six of her TV dramas airing on TVB. Of the six roles, Paris Yiu from Lives of Omission had garnered the most attention. For the role, Tsui was awarded a My Favourite TVB Female TV Character award from the StarHub TVB Awards, nominations in the Best Actress and Favourite Female Character categories for the TVB Anniversary Awards 2011, as well as a nomination for Outstanding Actress in Television by the Ming Pao Anniversary Award.

In 2009, Tsui starred in I Corrupt All Cops, a Hong Kong crime drama, directed by Wong Jing, who was impressed with the success of her debut performance in Eye in the Sky. Eason Chan, who plays Tsui's husband in the film, said Tsui's character is based on Shuang'er from Duke of The Deer and the Cauldron.

In 2008, Tsui took on her first villain role in Moonlight Resonance, and the role had earned her a Top 5 position in the Best Supporting Actress category of the TVB Anniversary Awards 2008. On the other hand, her leading role in Speech of Silence, in which she played a deaf character, had earned her a Top 10 position in the Best Actress category of the aforementioned awards show.

In 2007, Tsui had three TVB series released, including The Brink of Law, On the First Beat, and Steps. The roles cumulatively earned her the Most Improved Female Artist award from the TVB Anniversary Awards 2007. Her role in Steps also earned her nominations in the Best Actress category, as well Favourite Female Character category for the same awards show.

Aside from her development in television acting, Tsui also experienced success in developing her career in the film industry. In 2007, through a series of auditions, Tsui was cast as the female lead, alongside A-list actors Tony Leung Ka-fai and Simon Yam, in Eye in the Sky, which is a film produced by Johnnie To and directed by Yau Nai-hoi. With her performance in the film,

Eye in the Sky was praised by professional Hong Kong film critic, Sek Kei, as the best Hong Kong film in the first half of 2007. The film was subsequently entered into the Berlin International Film Festival, as well as the Shanghai International Film Festival. Through her performance in the film, Tsui was widely acclaimed to be talented in acting and a rising actress worth looking out for.

Following guest roles in The Zone and When Rules Turn Loose in 2005, Tsui made her official TV debut in TVB series, La Femme Desperado in 2006. Professional Taiwanese film critic, Mai Ruoyu, while critiquing Tsui's film performance, had said that Tsui had demonstrated strong charisma and had effectively held her own in La Femme Desperado, even while starring alongside veteran actresses, Sheren Tang and Melissa Ng. Her role as Ida in the series was also nominated in the Best Supporting Actress category, as well as the Favourite Female Character category, in the TVB Anniversary Awards 2006.

Kate Tsui Tsz-shan is a former Hong Kong actress, who is best known for her work with Television Broadcasts Limited (TVB), and to an extent, for her film work and singing career. She also holds the Miss Hong Kong 2004 title. In December 2019, she announced her retirement from the entertainment industry.

In 2004, she entered the Miss Hong Kong beauty pageant and was crowned the winner along with the titles of Miss Photogenic, Miss International Goodwill, and the Slimming Beauty Award. After the pageant, she had signed with TVB and began her career as an actress.