Viji's sister is actress Saritha, who was already a star when Viju made her debut as the sister of Rajinikanth's character in the 1981 comedy film Thillu Mullu by K. Balachander. Despite the film becoming a success, Viji chose to concentrate on her studies and refrained from acting until the 1990s.

Besides performing supporting roles in films including K. Balachander's Paarthale Paravasam (2001) as the sister of Raghava Lawrence and in Mani Ratnam's Aaytha Ezhuthu (2004) as the sister of Krishna's character, she mainly worked in television serials. In over 20 years, she was part of over 35 serials. In 2012, she played Nirmala, a vegetable vendor affected by bipolar disorder in Lakshmi Ramakrishnan's Aarohanam, and won critical acclaim for her performance.^[3][5] A critic from Sify.com noted: "in an author backed role, Viji Chandrasekhar steals the show as she is the pivot around which the film revolves."^[6]