Aruna Asaf Ali had a major role in Indian Independence Movement. She became a member of Indian National Congress after marrying Asaf Ali and participated in public processions during the Salt Satyagraha. She was arrested on the charge that she was a vagrant and hence not released in 1931 under the Gandhi-Irwin Pact which stipulated release of all political prisoners. Other women co-prisoners refused to leave the premises unless she was also released and gave in only after Mahatma Gandhi intervened. A public agitation secured her release. On 8 August 1942, the All India Congress Committee passed the Quit India resolution at the Bombay session. The government responded by arresting the major leaders and all members of the Congress Working Committee and thus tried to pre-empt the movement from success. Young Aruna Asaf Ali presided over the remainder of the session on 9 August and hoisted the Congress flag at the Gowalia Tank Maidan. This marked the commencement of the movement. The police fired upon the assembly at the session. Aruna was dubbed the Heroine of the 1942 movement for her bravery in the face of danger and was called Grand Old Lady of the Independence movement in her later years. Despite the absence of direct leadership, spontaneous protestsand demonstrations were held all over the country, as an expression of the desire of India’s youth to achieve independence. She was a member of the Congress Socialist Party, a caucus within the Congress Party for activists with socialist leanings. Disillusioned with the progress of the Congress Party on socialism she joined a newparty, Socialist Party in 1948. She, however, left that party along with Edatata Narayanan and they visited Moscow along with Rajani Palme Dutt. Both of them joined the Communist Party of India in the early 1950s. On the personal front, she was bereaved when Asaf Ali died in 1953.

In 1954, she helped form the National Federation of Indian Women, the women's wing of CPI but left the party in 1956 following Nikita Khrushchev's disowning of Stalin. In 1958, she was elected the first Mayor of Delhi. She was closely associated with social activists and secularists of her era like Krishna Menon, Vimla Kapoor, Guru Radha Kishan, Premsagar Gupta, Rajani Palme Joti, Sarla Sharma and Subhadra Joshi for social welfare and development in Delhi.