He was the son of the expatriate Eyre Evans Crowe, and brother of Eyre Crowe, a painter of historical subjects and genre, the friend and amanuensis of William Makepeace Thackeray. The elder Crowe was Paris correspondent of the London Morning Chronicle whose home, with a London interlude 1844–1851, was the centre of a liberal and artistic circle that mixed French and expatriates. During the Crimean War he was the correspondent of the Illustrated London News, and during the Austro-Italian War represented The Times in Vienna.
He was British consul-general in Leipzig from 1860 to 1872, and in Düsseldorf from 1872 to 1880, when he was appointed commercial attaché in Berlin, being transferred to Paris in 1882. In 1883 he was secretary to the Danube Conference in London; in 1889 plenipotentiary at the Samoa Conference in Berlin; and in 1890 British envoy at the Telegraph Congress in Paris, in which year he was made K.C.M.G.
During a sojourn in Italy, 1846-1847, he cemented a lifelong friendship with the connoisseur Cavalcaselle, who was forced to flee to London after the Revolutions of 1848 and moved in with Crowe. Together they produced several historical works on art of classic importance, notably Early Flemish Painters (London, 1857) and A New History of Painting in Italy from the Second to the Sixteenth Century (London, 1864-1871, 5 vols.). In 1877, he and Crowe issued a biography, Titian: His Life and Times (London, 1877) and. Raphael: His Life and Works (London, 1882–85). The division of labour in the partnership was seamless; though Crowe produced most of the final edited text, Cavalcaselle's eye and notes, and, in the age before photographic reproductions, his quick sketches of compositions, were essential.
In 1895 Crowe published Reminiscences of Thirty-Five Years of My Life. He died at Schloss Gamburg in Bavaria on the 6th of September 1896.
Crowe and Cavalcaselle's great History of Painting was under revision by Crowe up to the time of his death, and then by S.A. Strong (d. 1904) and Langton Douglas, who in 1903 brought out vols. i. and ii. of Murray's new six-volume edition, the 3rd vol., edited by Langton Douglas, appearing in 1909. A reprint of the original edition, brought up to date by annotations by Edward Huttons, was published by Dent in 3 vols. in 1909.