While connected with Oxford life he held the incumbency of the neighbouring church of Cowley, and near the close of his academic career, in 1801, he was nominated one of the preachers at Whitehall Chapel.

Through the influential support of Cyril Jackson, Carey was appointed to the head-mastership of Westminster School in January 1803, staying until December 1814.

On resigning his position at his old school he withdrew to his country living, residing there until 1820, when he was called to preside over the diocese of Exeter.

At Exeter he remained for ten years, when he was translated to St Asaph, being elected to his new see on 12 March 1830 and confirmed on 7 April.

He died at his house in Portland Place, London, on 13 September 1846, but his body was carried into Wales and buried in the churchyard of St, Asaph Cathedral on 2 October 1846.