In the late 1810s and early 1820s Martin had experimented with various printmaking techniques. In 1824 he mastered mezzotint and received an extraordinarily lucrative commission to produce mezzotint illustrations to John Miltonís epic poem Paradise Lost. He now concentrated on printmaking rather than oil painting as a means of making money out of his art.

The Paradise Lost prints were applauded for their technical invention and poetic power. Although mezzotint was traditionally used as a way of reproducing paintings, Martinís prints were original compositions and were marketed as having Ďall the spirit and finish of the Painterís touchí. The prints were sold across the world, and Martinís fame and influence spread.

Martin went on to produce large separate mezzotints of biblical scenes and ventured a new, self-published series illustrating the Bible. The latter faltered, and Martinís attempt to establish himself as an independent publisher ultimately failed. Although he largely gave up printmaking by around 1837, his creative use of mezzotint is now generally considered as his central achievement as an artist.