He was educated at Rugby School under Thomas Arnold.
In June 1846 Shirley matriculated at University College, Oxford, but in the following year he migrated to Wadham College, where he had gained a scholarship. He obtained a first class in the honour school of mathematics in 1851, and in 1852 was elected a Fellow of his college. He had to vacate his fellowship three years later, on his mother"s death, when he inherited a small landed property.
From 1855 to 1863 he was tutor and mathematical lecturer of Wadham.
lieutenant was during this period that he began historical study. In May 1863, he preached in the university church a sermon on the unreasonableness of Arnold"s teaching.
Later that year he was made regius professor of ecclesiastical history and canon of Christ Church, Oxford. He was one of the pioneers of the university extension movement, and played a part in the founding of Keble College.
His career was cut short at the age of thirty-eight.
He died on 20 November 1866. Alice Shirley (17 June 1856 – 18 January 1911), married William Richardson Linton Lady Mary Philippa Shirley (28 December 1857 – 9 September 1917) Walter Sewallis Shirley (13 October 1859 – 21 January 1861) Lady Laeta Shirley (29 June 1861 – 27 November 1928) Walter Shirley, 11th Earl Ferrers (1864–1937) Honorary
His closest friend at school and throughout his life was his cousin, William Henry Waddington, later in French politics. His theological views underwent considerable change. The position which Shirley occupied at the time of his death was still a provisional one.