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A Modern Churchman, Bethune-Baker was known for his work on the person and writings of Nestorius. He was co-editor of the Journal of Theological Studies. He was a Fellow of Pembroke College, Cambridge for sixty years. His funeral service took place in Pembroke College Chapel on 17 January 1951, but he was buried in the Ascension Parish Burial Ground, Cambridge. He was a cousin of Arthur Christopher Benson, who is also buried in the Ascension Parish Burial Ground.
He was married to Edith Bethune-Baker, née Furneaux Jordan, a welfare campaigner, who was born in 1862. Their son Arthur Bethune-Baker was a contemporary of Charles Hamilton Sorley at Marlborough College, but he died while still at school, aged sixteen.
- Influence of Christianity on War, 1888
- The Meaning of Homoousios in the "Constantinopolitan" Creed, 1901.
- An Introduction to the Early History of Christian Doctrine, to the Time of the Council of Chalcedon, 1903 (revised 1933)
- Nestorius and His Teaching, 1908.
- The Faith of the Apostles' Creed: An Essay in Adjustment Of Belief and Faith, 1918.
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