In 1805 Pye was entrusted by Heath with the execution of a plate of Inveraray Castle from a drawing by J. M. W. Turner.
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In 1830, at the request of John Sheepshanks, he undertook the publication of a series of engravings from pictures in the National Gallery during the 1830s.
The son of a Sheffield bookseller, Pye-Smith was surrounded by books in his youth and was practically self-taught: he did take Latin lessons from Jehoiada Brewer.
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He married secondly in 1801 Martha Corbett, by whom he had a son Henry John Pye, who in 1833 inherited the Clifton Hall, Staffordshire estate of a distant cousin and who was High Sheriff of Staffordshire in 1840.