Vasundhara Das was born into a Tamil speaking Hebbar Iyengar Brahmin family in Bangalore. She studied at Cluny Convent High School, Bangalore, Sri Vidya Mandir, Bangalore and Mount Carmel College, Bangalore, graduating in Economics, Statistics and Mathematics. She began training in Hindustani classical music under her grandmother Indira Das and later trained under Lalita Kaikini and Pandit Parameshwar Hegde. In her college days, she was a lead singer of a girl band and soprano in the college choir. In an interview, she states that-"I got booed off the first time I sang on stage". She is multilingual and speaks Tamil, Kannada, Hindi, Spanish and English. Vasundhara married her long-time friend, Roberto Narain, a drummer. She started her playback singing career with A. R. Rahman's Tamil film Mudhalvan, for which she sang the song "Shakalaka Baby". She also played the female lead role opposite Ajith in the Tamil movie Citizen (film).
She has sung one song for maestro Ilaiyaraaja, pattu viral thottu vittadhaal, in the Tamil movie Dhanush directed by A M Gurumani. She has sung a song in 'Lagaan' for the British character played by Rachel Shelley. She is also renowned for Kattipudi, Kattipudi da from the movie Kushi. She often sings for the actress Preity Zinta among others.