The effects of coverage layer and temperature on the tensile properties and surface microstructure of H62 brass subjected to laser shock peening (LSP) were systematically investigated. Ultimate tensile strength, elongation rate, and in-depth microstructural evolutions of three kinds of LSPed specimens, including LSPed specimens with one coverage layer and three coverage layers at room temperature, and one coverage layer at dynamic strain aging temperature, were subsequently measured and characterized. Special attentions were paid to surface nanocrystallization and amorphization of H62 brass subjected to room-temperature LSP and warm LSP technologies for the first time. The formation mechanisms of surface nanocrystallization and amorphization induced by room-temperature LSP and warm LSP were also discussed and completely revealed, and surface nanocrystallization contributed to the improvement of ultimate tensile strength and elongation rate of H62 brass subjected to LSP.