This study describes the geological characteristics of gold mineralization along the Cape Ray Fault Zone, which hosts one of the most important vein-type gold deposits in the Appalachians. The study focuses on the lithological and structural control of the mineralization and its relationship with the structural evolution of the fault zone. It is based on detailed lithological and structural analyses and radiometric dating along a 60-kilometre segment of the Zone as well as on a detailed mineral deposit study of the gold mineralization within the Zone. The study documents a continuum of deformation from the Late Silurian to Early Devonian and demonstrates the origin of the mineralization as well as the controls on the development and geometry of the auriferous zones.