The Indian National Congress selected him General Secretary, in 1929 & 1934 and Member of the Working Committee for 12 years, from 1928-1940. When Ganhiji returned from South Africa, he actively participated in his programmes of Khadi and Village Industries and from Non-co-operation Movement of 1920, to the Quit India Movement of 1942. He was in jail several times and sustained a bullet injury in the firing in Karachi in the Salt Satyagraha Movement in 1930.

Jairamdas Doulatram was also very close to Sardar Patel and Rajendra Prasad. In 1926, he was elected to Bombay Legislative Council and in 1946; he became member of the constituent Assembly. He was appointed the Governor of Bihar on 15th August 1947, after India's Independence and in 1948, became Union Minister of Food & Agriculture. From 1950 to 1955, he was Governor of Assam and during this period, he did research in history, customs and culture of the tribal people. He was also the Editor of Sindhi national journal, "The Hindu", "The Hindustan Times" (Delhi) and Gandhiji's weekly, "The Young India". In 1957, he became the Chief Editor of "Collected Works of Mahatma Gandhi".