[3] Smith was ordained a deacon on 19 June 1859 and priest on 3 Jun 1860;[1] he was vicar of Trumpington, 1867–69, and principal of St Aidan's Theological College, 1869-90.

He was consecrated bishop of Sydney and Primate of Australia at St Paul's Cathedral, London, on 24 June 1890, and became archbishop in 1897.

There was some advance in education; Moore Theological College was reopened, and the Church of England Grammar School For Girls was established in his period.

Though an extreme evangelical he was broadminded and an advocate for the union of the churches; and though essentially a man of peace, he spoke strongly against gambling and other evils.

Smith had a dislike of ceremonial, a passion for accuracy, and was a fine scholar and linguist, interested also in astronomy and botany.