In 1782 he became fellow of King's College, Cambridge, and took orders, receiving the living of Holy Trinity, Cambridge, in the following year. He was at first so unpopular that the services were frequently interrupted, and he was often insulted in the streets. Having lived down this prejudice, he subsequently gained a very remarkable and lasting influence among the undergraduates of the university.
He became a leader among evangelical churchmen, was one of the founders of the Church Missionary Society, and acted as adviser to the East India Company in the choice of chaplains for India. His chief work is a commentary upon the whole Bible, entitled Horae homileticae (London, 1819-1820). The "Simeon Trustees" were instituted by him for the purpose of acquiring church patronage in the interests of evangelical views.
See Memoirs of Charles Simeon, with a selection from his writings and correspondence, edited by the Rev. W Carus (3rd ed., 1848); HCG Moule, Charles Simeon (London, 1892).