A low carbon structural steel was surface-hardened by friction stir processing (FSP) through 4 mm thickness from the surface. The hardness of the alloy increased from 140 Hv0.1 to about 240 Hv0.1 after single-pass FSP. This improvement came from the substantial microstructural refinement due to both severe plastic deformation and dynamic recrystallization. Both yield and tensile strength of the alloy increased without a considerable decrease in ductility after FSP. Friction and wear behavior of the alloy before and after FSP was investigated by a pin-on-disk type tribometer according to ASTM-G133. The substantial increase in both hardness and yield strength resulted in a considerable improvement in wear resistance of the alloy depending on applied pressure. In this study, metallurgical and mechanical reasons for such improvement in wear behavior and any change in wear mechanisms after FSP were investigated.