Purey-Cust became the Archdeacon of Buckingham in June 1875, and installed Vicar of Aylesbury in the same year. His final appointment was as Dean of York from 1880 to 1916.

For the next 36 years, Purey-Cust meticulously catalogued York Minster's heritage and was the author of Heraldry of York Minster, 1890. He died in office in his 88th year and is commemorated by a mural monument