Sarla Devi's family was a follower of Brahmoism, a religion founded by Ram Mohan Roy and later developed by Sarala's grandfather Debendranath Tagore.

During anti partition agitation she spread the gospel of nationalism in Punjab and maintained secret revolutionary society.

A year later, she returned home and started writing for Bharati, a Bengali journal, while also beginning her political activities.

[5] From 1895 to 1899, she edited Bharati jointly with her mother and sister,[6] and then on her own from 1899 to 1907, with the goal of propagating patriotism and to raise up the literary standard of the journal.

[7] With several branches around the country, it promoted education and vocational training for women without consideration of class, caste and religion.

[3] In 1905, Sarala Devi married Rambhuj Dutt Chaudhary (1866–1923), a lawyer, journalist, nationalist leader and follower of Arya Samaj, the Hindu reform movement founded by Swami Dayananda Saraswati.

When her husband was arrested for his involvement in Non-cooperation movement, Mahatma Gandhi visited her home in Lahore as a guest.

[3] After her husband's death in 1923, Sarala Devi returned to Kolkata, and resumed editing responsibilities for Bharati from 1924 to 1926.

[3] Her autobiography Jivaner Jhara Pata was serialized in Desh, a Bengali literary magazine, during the later period of her life, in 1942–1943.