She appeared in two films in 2008; Honganasu, her first Kannada project and Aayudham Seivom in Tamil. The latter, which featured her as the female lead opposite Sundar C., was panned by critics and she was criticized for accepting that role, with reviewers noting that she had nothing to do in the film, "except roll her eyes". She next played Kani, a fiery, independent sales girl in a textile showroom in Angadi Theru (2010) that released two years after her last venture. The Vasanthabalan-directed tragedy drama focussed on the lives of young employees who work in retail department stores. The film was shot in real location at the Ranganathan Street in T. Nagar, Chennai with hidden cameras, with Anjali disclosing that they wore the uniform of a particular textile company, passing off as real salepeople and selling goods. Angadi Theru opened to rave reviews, whilst also fetching Anjali critical acclaim for her performance, who went on to bag several accolades, including the Filmfare Award for Best Actress - Tamil.She subsequently appeared in two family drama films; S Pictures' Rettaisuzhi, in which she shared screen with veteran directors Bharathiraja and K. Balachandar, and Magizhchi, co-starring and directed by Gowthaman. The latter released to favorable reviews, and Anjali received positive feedback on her performance, being labelled as "impressive", and "almost perfect as the young, a bit mischievous, village girl"; however both films failed to succeed at the box office.

In 2011, she first appeared in Payyans alongside Jayasurya, which marked her debut in Malayalam cinema, followed by a lead female role in the Cloud Nine Movies-production Thoonga Nagaram, in which she starred as an anchor in local television,and a cameo appearance in a song in Ko that also featured other lead actors from Tamil cinema. She was then seen in the small-budget drama film Karungali, directed by Mu. Kalanjiyam. Kalajiyam had signed up Anjali, rechristening her as Sundari then, for a film titled Sathamindri Muthamidu, even prior to Kattradhu Thamizh, followed by three more films, all of which were cancelled.Following her rise to fame post Angadi Theru, Kalanjiyam revived one of the projects, namely Karungali, with Anjali agreeing to part of it, owing to her prior commitments. The film featured her as a childless housewife living in an unharmonius relationship with her husband, and was a critical and commercial failure. While starring in Thoonga Nagaram, she was offered a minor supporting role in another project of the production studio, Mankatha.The Ajith Kumar-starrer, directed by Venkat Prabhu, was Anjali's first high-budget project and featured her as part of an ensemble cast. The film emerged a financial success and Anjali's highest-grossing film in her career, however her role in the film was small and not well received generally. Meanwhile, she was casted by director A. R. Murugadoss to perform a lead role in his maiden production Engeyum Eppodhum alongside Jai, Sharvanand and Ananya, directed by his assistant M. Saravanan. Anjali essayed the role of a bold and dominating nurse, with critics again heaping praise on her performance. The Hindu wrote that she "has given her best [and] steals the show in the climax" while Rediff's Pavithra Srinivasan cited it was her "who clearly walks away with the honours", adding that "the extent of her feelings emerges only at the end, and carries you away" and calling it a "notewothy performance".Moreover, Vasanthabalan's period piece Aravaan would feature her in a cameo appearance, while she has also signed to be part of Sundar C's next directorial, Masala Cafe.