In 1853 he went up to Cambridge, earning the degrees of Bachelor of Arts in 1857, then Master of Arts in 1860 from Clare College, Cambridge. In 1864, he became the curate at Horbury Bridge, West Yorkshire. It was while acting as a curate that he met and fell in love with Grace Taylor, the 16-year-old daughter of a mill hand. He sent Grace to live for two years with a vicar's family in York to learn proper manners, then brought her back and married her in 1868 at Wakefield. Their marriage lasted for 48 years, and the couple had 15 children, all but one of whom lived to adulthood. When he buried his wife in 1916 he had carved on her tombstone the Latin motto Dimidium Animae Meae ("Half my Soul").
In 1880 he inherited the family estates of Lewtrenchard, Devon, which comprised 3,000 acres (12 km²) and in 1881 he installed himself at Lewtrenchard as both Squire and Parson. He did a great deal of work restoring St. Peter’s Church, Lewtrenchard, and his home Lewtrenchard Manor.
Baring-Gould and Sheppard produced a second collection called A Garland of Country Songs in 1895. A new edition of Songs of the West was proposed for publication in 1905. Sheppard had died in 1901 and so the collector Cecil Sharp was invited to undetake the musical editorship for the new edition. Sharp and Baring-Gould also collaborated on English Folk Songs for Schools in 1907. This collection of 53 songs was widely used in British schools for the next 60 years.
Though he had to modify the words of some songs which were too rude for Victorian ears, he left his original manuscripts for future students of folk song. His work preserved many beautiful pieces of music and their lyrics which otherwise might have been lost.
The folk-song manuscripts from Baring-Gould's personal library and from public libraries have been published as a microfiche edition available for study in the main Devon Libraries and other places (including the Vaughan Williams memorial Library in London). Thirty boxes of unpublished manuscript material on other topics (the Killerton manuscripts) are kept in the Devon Record Office in Exeter. The folksong manuscripts, including the notebooks used in the field, given to Plymouth Public Library were deposited with the Plymouth and West Devon Record Office in 2006.
Cecil Sharp dedicated his English Folk Song—Some Conclusions to Baring-Gould.
Baring-Gould wrote many novels (including Mehalah), a collection of ghost stories, a 16-volume The Lives of the Saints, and the biography of the eccentric poet-vicar of Morwenstow, Robert Stephen Hawker. His folkloric studies resulted in The Book of Were-Wolves (1865), one of the most frequently cited studies of lycanthropy. Half-way through, the topic changes to crimes only vaguely connected to werewolves, including grave desecration and cannibalism.
One of his most enduringly popular works was Curious Myths of the Middle Ages , first published in two parts in 1866 and 1868, and republished in many other editions since then. "Each of the book's twenty-four chapters deals with a particular medieval superstition and its variants and antecedents," writes critic Steven J. Mariconda. H. P. Lovecraft called it "that curious body of medieval lore which the late Mr. Baring-Gould so effectively assembled in book form.
Baring-Gould served as President of the Royal Institution of Cornwall for ten years, starting in 1897.
Stories of his own eccentricity have been exaggerated. He did for a time, have a bat in his care while he was teaching at Hurstpierpoint. More usually it lived in an old sock in his room, where its life was ended when a housemaid stepped on it. It is also told how, at a children's party he asked a small girl, "And whose little girl are you?" whereon she burst into tears, and said: "I'm yours, Daddy." This story was verified by his daughter, Joan, who said that the little girl was her.
One grandson, William Stuart Baring-Gould, was a noted Sherlock Holmes scholar who wrote a fictional biography of the great detective—in which, to make up for the lack of information about Holmes's early life, he based his account on the childhood of Sabine Baring-Gould. Sabine himself is a major character in Laurie R. King's Sherlock Holmes novel The Moor, a Sherlockian pastiche. In this novel it is revealed that Sabine Baring-Gould is the godfather of Sherlock Holmes.