Not long after he was born, his father died and the family moved to England. In 1801, Wolfe was sent to a school in Bath but was sent home a few months later due to his ill health. From 1802 to 1805, he was tutored by a Dr Evans in Salisbury before being sent to Hyde Abbey School, Winchester. He seems to have been exceedingly popular both at school and within his own family. In 1808, his family returned to Ireland, and the following year he was entered into Trinity College, Dublin, graduating in 1814. He had turned down the chance to read for a scholarship as he was in love with a girl and could not commit to celibacy as was then required.

Charles Wolfe is best remembered for his poem, “The Burial of Sir John Moore after Corunna”, written in 1816 and much collected in 19th and 20th century anthologies. The poem first appeared anonymously in the Newry Telegraph of 19 April 1817, and was re-printed in many other periodicals. But it was forgotten until after his death when Lord Byron drew the attention of the public to it. Wolfe’s only volume of verse, Poetical Remains appeared in 1825 with “The Burial of Sir John Moore” and fourteen other verses of an equally high standard.

He was ordained as a Church of Ireland priest in 1817, first taking the Curacy of Ballyclog in County Tyrone before transferring almost immediately to Donaghmore, County Tyrone. There he developed a close friendship and deep respect for the Rev. Thomas Meredith, Rector of nearby Ardtrea, and a former Fellow of Trinity College Dublin. Wolfe wrote two epitaphs for Meredith, one on his memorial in the parish church of Ardtrea, and another intended for his tomb, which can both be read within Meredith’s entry.