Athersmith played a key role in Villa's title-winning sides of 1894, 1896, 1897, 1899 and 1900 as well as reaching three FA Cup finals, finishing on the losing side in 1892 before gaining winners' medals in 1895 and the Double-winning final of the 1896–97 season. He was also a member of the team that were victims of a giant-killing in the 1899–1900 FA Cup at the hands of Millwall Athletic.