Zhang appeared in a minor, uncredited role in the 2007 film The Longest Night in Shanghai. Stephen Chow first noticed her in an advertisement for Kentucky Fried Chicken, and recruited her into his agency. Zhang was given arduous training in acting, dancing, and singing. She made her debut in the science fiction film CJ7, playing a young Teacher. The role brought her major media attention, and because of Chow's tradition of starring alongside new actresses who later gain other major roles, Zhang has been called one of the "星女郎" (xīng nǚ láng, "star girls" or "Sing girls"—Sing Yeh is a Common nickname of Chow's).

Zhang then starred in the romantic comedy All About Women playing a headstrong Business woman. In 2009, she played a country girl with a passion for hip-hop music in Jump, a musical comedy directed by Stephen Fung and penned by Stephen Chow.

In 2012, Zhang was cast in the role of Qian Xuesen's wife, Jiang Ying in the biopic of the author. She then starred in the film adaptation of the Chinese literary classic White Deer Plain written by Chen Zhongshi. She plays Tian Xiao'e, a sensual, illiterate woman who follows her instincts. The role posed a challenge to Zhang, as it involve various intimate scenes, and many other actresses have rejected the role. Zhang won her first "Best Actress" trophy at the Chinese American Film Festival. She was also voted the Most Popular Actress at the Beijing College Student Film Festival for her performance.

Zhang Yuqi and Wang Quan'an had a whirlwind romance in 2011, and they married on April 18 in that year. But Zhang has announced they were divorced on July 2, 2015.

Zhang married businessman Yuan Bayuan in October 2016.

In 2017, Zhang starred in the fantasy comedy film The Golden Monk directed by Wong Jing. The same year, she starred in Chen Kaige's fantasy mystery film Legend of the Demon Cat. Zhang won the Best Supporting Actress award at the Asian Film Awards for her performance.