From 1856 to 1860 he was the Curate of Drinkstone and Creeting St Peter, both in Suffolk, but in 1860 he was appointed Rector of Drayton Beauchamp, a living he occupied until his death in 1883.
He obtained a BA degree from Trinity College, Cambridge in 1851 and an MA in 1855[1] In 1857 his father was the rector of Breadsall in Derbyshire, a small village which also included the naturalists Joseph Whittaker and Francis Darwin.
In 1846 Harpur-Crewe and Whittaker reported on the earlier local extinction from Derbyshire of the lady's slipper orchid Cypripedium calceolus.
[3] Whittaker's plant collecting activities began to decline around 1863 at about the time Crewe moved away to take up the position of rector in the parish of Drayton Beauchamp in Buckinghamshire.
In 1877 Harpur-Crewe reported on a visit he made to Tresco in the Scilly Isles where he commented on the insects which was where "all the plants of Australia, the Cape, New Zealand, &c., flourish with almost native luxuriance.