[9] She completed her schooling in Razole and later moved to Chennai where she continued her studies, pursuing a degree in mathematics.Anjali remarked that her parents had aspirations to become an actor and that they "realised their dreams" through her.

During one of her modelling assignments, she was spotted by director Siva Nageswara Rao, who offered her a starring role in his Telugu thriller film Photo (2006).

Anjali won critical praise for her portrayal of Anandhi, the childhood friend and love interest of a young teacher-turned-psychopath (enacted by Jeeva).

[14] Her performance earned her the Vijay Award for Best Debut Actress for that year,[15] and she grew in popularity, leading her to several more offers, albeit the film proved commercially unsuccessful.

The latter, which featured her as the female lead opposite Sundar C, was panned by critics and she was criticised for accepting that role, with reviewers noting that she had nothing to do in the film,[17] "except roll her eyes".

[10] Angadi Theru opened to rave reviews, whilst also fetching Anjali critical acclaim for her performance, which went on to win several accolades,[22] including the Filmfare Award for Best Actress – Tamil.

[23] She subsequently appeared in two family drama films; S Pictures' Rettaisuzhi, in which she shared screen with veteran directors Bharathiraja and K Balachandar,[24] and Magizhchi, co-starring and directed by Gowthaman.

The latter released to favourable reviews,[25] and "almost perfect as the young, a bit mischievous, village girl";[26] however both films failed to succeed at the box office.

Following her rise to fame post Angadi Theru, Kalanjiyam revived one of the projects, namely Karungali, with Anjali agreeing to be part of it, owing to her prior commitments.

Meanwhile, she was cast by director AR Murugadoss to perform a lead role in his maiden production Engaeyum Eppothum alongside Jai, Sharwanand and Ananya, directed by his assistant M Saravanan.

[38] The Hindu wrote that she "has given her best [and] steals the show in the climax",[39] while Rediff's Pavithra Srinivasan cited it was she "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 "noteworthy performance".

In Tamil, she starred in Karthik Subbaraj's Iraivi where her performance as the happy go lucky girl turned long suffering wife of Vijay Sethupathi gave her critical acclaim and audience appreciation.

Though the film had an average return at the box office, she garned a nomination for Best Performance in a Leading Role- Female (Tamil) at the 2nd IIFA Utsavam.

[50][51] In December 2017, her film with Jai & Janani Iyer titled Balloon directed by newcomer Sinish had a moderate-average performance at the box office.

[52] She signed a Tamil film Peranbu (2019) opposite Mammootty directed by Ram, where her performance was overshadowed by Mammooty and Baby Sandhana.