Moyle attended Yale University, where he played football as an end. He graduated in 1891, and then took over as the head football coach at Lafayette College. Moyle served in that position for two years and amassed a record of 7–16–1. In 1893, Moyle became the first "all-season head coach" at Dartmouth College and posted a 9–7 record during his two-year tenure. The Indians' losses to Harvard, 16–0, and Yale, 28–0, were seen as evidence of improvement under Moyle. By comparison, Yale had routed Dartmouth, 113–0, in 1884, which marked the beginning of the so-called "Yale jinx". Dartmouth was awarded the Triangular Football Conference championship in both years of Moyle's tenure. In 1895, Moyle moved on to Brown University, where he amassed an 18–15–2 record over three years as head coach.