In 1853 he travelled to Morocco, where for the following ten years he produced many of his most famous paintings depicting scenes of the world he encountered. Dehodencq was the first foreign artist known to have lived in Morocco for an extended number of years.
While he considered himself to be a Last of the Romantics, his work is generally categorized with the mid-19th-century Orientalist artistic movement.
Dehodencq married Maria Amelia Calderon in 1857 in Cadiz, Spain, and they had three children. Their son, painter Edmond Dehodencq, was born in Cadiz in 1860 (and died in Paris in 1887). Dehodencq returned to Paris in 1863 with his wife, and was decorated with the Legion of Honour in 1870. He committed suicide on 2 January 1882 having been sick for a long time and is buried in the Montmartre Cemetery.