Based on strain-induced grain refinement, a novel surface mechanical attrition treatment (SMAT) technique has been developed to synthesize a nanostructured surface layer on metallic materials in order to upgrade their overall properties and performance without changing their chemical compositions. In recent several years, the microstructures and properties of surface layer were systematically investigated in various SMAT metals and alloys, including b.c.c., f.c.c. and h.c.p. crystal structures. Different grain refinement approaches and nanocrystalline formation mechanisms were identified in these deformed materials, involving dislocation activities, mechanical twinning and interaction of dislocations with mechanical twins. The properties of the surface layer were measured by means of hardness, tensile, fatigue and wear tests. The enhanced properties of the surface layer are mainly attributed to the strain-induced grain refinement. In this work, we reviewed the microstructures and properties of surface layer in the SMAT materials.