Mundassery entered politics through the Kochi Prajamandalam and was elected as a Member of the Legislative Council (MLC) of the princely state of Cochin in 1948 from the constituency of Aranattukara.
Through his controversial theory about Rooparbhadrata – formal excellence – Mundassery ushered in a new chapter of literary hermeneutics, which was unheard of in Malayalam until then.
To a great extent, the proposed bill directly led to the snowballing of the Vimochana Samaram and the subsequent downfall of the E.M.S.
As the Education Minister of the first democratically elected ministry of the newly formed State of Kerala, Mundassery was instrumental in the establishment and restructuring of some of the early universities and prime educational institutions of the state, having had experience as the Vice Chancellor of the Cochin University of Science and Technology.
Mundassery was the guru of many pupils at St. Thomas College, Trichur, among whom were some of the future leaders of Kerala such as C. Achutha Menon and Mathai Manjooran.