Anjali Devi started her career as a theatre artist before coming into movies. She made her debut with the film Raja Harishchandra in 1936 as a child artist. It was C.Pullayya, who discovered her and gave her the chance to star as a lead actress Mohini in the film Gollabhama in 1947. This movie made her an overnight star and she eventually ended up acting in over 350 films.
Few years later she tried her hands at production in 1955 with the film Anarkali, in which she herself acted. As a producer she produced some 27 films. She was an avid admirer of Sathyasai Baba and thus produced a Television serial on Sathyasai Baba.
In her personal life she married to P. Adinarayana Rao, who was a noted music director in the year 1940.The couple settled in Chennai with their two sons. They had their own production house and produced several Telugu films under the banner, Anjali Pictures.
She passed away in 2014 at Vijaya hospital, Chennai.