Smitha Rajan started her dance training at her maternal grandparents' residence in Tripunithura near Kochi.

Smitha's aunt, Kala Vijayan (a recipient of the Kerala Sangeetha Nataka Akademi Award for Mohiniyattam) was the first to notice talent in young Smitha during a master class at her grandparents' institution, Kerala Kalalayam in Tripunithura.

[2] Her grandfather, Kalamandalam Krishnan Nair, taught her Kathakali and fine-tuned her Mukha abhinaya (facial expressions).

Smitha has performed with many classical dancers from India in dance styles such as Bharatanatyam, Odissi, and Kuchipudi.

[8] She produced as well as appeared in the 2019 documentary on Kalamandalam Kalyanikutty Amma titled "Mother of Mohiniyattam," which was directed by Dr. Vinod Mankara.