After his marriage to Uttara Chaudhury, daughter of freedom fighter parents, Nabakrushna Chaudhury and Malatidevi Chaudhury, the young couple moved to Vedchhi, a tribal village 60 km from Surat in Gujarat, to work as teachers in a Nai Taleem school. Following the Bhoodan (land gift) movement launched by Vinoba Bhave, Narayan traversed through the length and breadth of Gujarat, by foot, collecting land from the rich and distributing the same among the poor landless villagers. He started the mouthpiece of Bhoodan movement, titled Bhoomiputra (Son of the Soil) and remained its editor till 1959.

Narayan joined the Akhil Bharatiya Shanti Sena Mandal (Indian Peace Brigade), founded by Vinoba and headed by veteran socialist leader Jayaprakash Narayan (widely known as "JP"). As the general secretary of the Shanti Sena, Narayan recruited and trained peace volunteers throughout the country who intervened during ethnic conflicts and helped establish harmony among conflicting communities.

Narayan was involved in the setting up of Peace Brigades International and was elected as the chairman of the War Resisters' International. He along with a Pakistani peace group were awarded the UNESCO prize for International Peace.

Narayan was active in the campaign against the imposition of emergency in India and brought out a magazine defying the censorship laws. As a close associate of JP, Narayan played an important role in helping the newly formed Janata Party, a conglomeration of major non-Congress political parties in India, arrive at a consensus on the name of Morarji Desai as the Prime Minister.

Following JP's death, Narayan moved to Vedchhi and set up the Institute for Total Revolution. The Institute imparts training in non-violence and Gandhian way of life. Narayan, as a way of paying tribute to his father, Mahadev Desai, wrote a four-volume biography of Gandhi in Gujarati, a dream his father could not fulfil in his lifetime because of his sudden death in prison on 15 August 1942.

Narayan was greatly pained by the genocide of Muslims in Gujarat carried out by Hindu fanatics in 2002 and decided to spread the message of harmony, peace and non-violence through the folk medium of narrating the story of Gandhi's life and times. Narayan's Gandhi Katha, delivered over a week, has been drawing large attendance in all major cities and towns of Gujarat.

Narayan was accorded the Sahitya Akademi Award for Gujarati in 1993 for the biography of his father Mahadev Desai he wrote as part of the centenary celebrations of Gandhi's close aide. Earlier, Narayan's book about his childhood reminiscences of Gandhi too had won the Sahitya Academy Award.