After studying at Eton College and Cambridge University, he was ordained as a priest in 1877, and was a curate at St Mary's in Reading.

[7] He made a second appearance for the MCC that summer, as part of a side which beat a Worcestershire team containing two of his brothers by three wickets.

[9] He was described in Scores and Biographies as being "Like the rest of the family he is a fine free hitter, and an excellent field at long-leg, or middle-wicket-off.

He began his career with a curacy at St Mary's, Reading, and in 1879 became a tutor at Keble College, Oxford, a post he retained until 1882.

[1] In 1882 Lyttelton moved with his wife to Cambridge to take up the post of first master of Selwyn College.

Initially, they made do with a suite of adapted student rooms until the Master's Lodge was built.

[11] Lyttelton's moderate political views along with his political connections to the prime minister (his aunt was Gladstone's wife,[12] and his brother served as his private secretary[1]) helped ensure acceptance of the new institution within the university.

He was described in a history of the college as a "fine teacher and a reserved, aloof-seeming man of judgement, decision and piety.