After making her debut as a supporting actress, she has been seen in lead roles in films including Vanmam (2014) and Baby (2015).
She consequently finished her schooling in Kendriya Vidyala Meenambakkam and followed that up with a BBA and MBA at Vels University in Chennai.
During her time in college, Anjali Rao became involved in modelling and worked on commercials which gave her an entry into the film industry.
Anjali Rao began her career playing supporting roles in films, notably appearing in the Nithya Menen-starrer Malini 22 Palayamkottai (2014), as Vijay Sethupathi's pair in the village drama Vanmam (2014) and as a ghost in the horror film Baby (2015).
She later worked with Gautham Vasudev Menon in Achcham Yenbadhu Madamaiyada (2016), featuring as Silambarasan's sister.