Laser shock peening (LSP) is a robust surface treatment technique widely exploited by industries of the modern era. In this study, aluminium 6061 alloy was treated with LSP at different power densities, and properties like hardness, surface roughness, microstructural evolution, and tribological behaviour were investigated. LSP applied at 3 GW/sq. cm raised the hardness and surface roughness to 97.1 HV and 0.499 μm, respectively, due to a fine-grained microstructure averaging 4.12 μm. Formation of a strain-hardened layer with dense dislocations improved the tribological performance of the LSPed specimens with minimal wear at 5 N load.