He enrolled as an advocate in Calcutta High Court in 1924, the same year in which his father had died. Subsequently, he left for England in 1926 to study at Lincoln's Inn and was called to the English Bar in the same year. In 1934, at the age of 33, he became the youngest Vice-Chancellor of the University of Calcutta; he held the office until 1938. During his term as Vice-Chancellor, Rabindranath Tagore delivered the University Convocation Address in Bengali for the first time, and the Indian vernacular was introduced as a subject for the highest examination. On 10 September 1938, the Senate of Calcutta university resolved to confer honorary D. Litt. on the Ex-Vice Chancellor in its opinion "by reason of eminent position and attainments, a fit and proper person to receive such a degree." Mukherjee received the D.Litt from Calcutta University on 26 November 1938.