A student at King’s College, London, and Girton College, Cambridge in the early 1890s, and a writer of precocious if imitative verse, Naidu was feted in London in the 1900s as the poet of an exoticized India.

From a Bengali family based in Hyderabad, Naidu was sent to Britain in 1895 on the Nizam's scholarship on the strength of her poetry. She was then not married and known as Sarojini Chattopadhyaya. However, she had already embarked on a romantic relationship with Dr Govindarajalu Naidu, in Hyderabad, who had studied medicine at Edinburgh; her father, Aghorenath Chattopadhyaya had also been a student at Edinburgh University.

She became the ward of Elizabeth Manning, the Secretary of the National Indian Association, whose step-mother had been involved in the foundation of Girton College, Cambridge. Naidu was heavily influenced by the poets Edmund Gosse, Arthur Symons and W. B. Yeats. Particularly interesting accounts of her very early Europeanized work appear as the introductions to her second and third collections, by Arthur Symons, and Edmund Gosse respectively. Her poetry also appeared in the Savoy. Appearances and readings by Naidu in the 1900s were reported in the Indian Magazine.

Naidu returned to India in 1898, beset by ill-health, that dogged her throughout her life. She maintained correspondence with poets in Britain but also embarked on a political career. Her returns to Britain were marked by poetry readings and receptions, convalescence in British nursing homes, as well as political rallies and meetings. She joined the Indian National Congress in 1904 and was vocal about women's rights. She gave evidence in 1919 to a Select Committee in favour of the women's vote in India. She also had a public confrontation with Edwin Montagu over the Amritsar Massacre. Naidu had met M. K. Gandhi in London in 1914 and became very close to him. She accompanied him on the famous Dandi salt march and accompanied him to the Round Table Conference in 1931. Naidu was appointed Governer of United Provinces in 1947 and died in office in February 1949.