Periodic nanostructures have wide applications in micro-optics, bionics, and optoelectronics. Here, a laser interference with subsequent etching technology is proposed to fabricate uniform periodic nanostructures with controllable morphologies and smooth surfaces on hard materials. One-dimensional microgratings with controllable periods (1, 2, and 3 μm) and heights, from dozens to hundreds of nanometers, and high surface smoothness are realized on GaAs by the method. The surface roughness of the periodic microstructures is significantly reduced from 120 nm to 40 nm with a subsequent inductively coupled plasma (ICP) etching. By using laser interference with angle-multiplexed exposures, two-dimensional square- and hexagonal-patterned microstructures are realized on the surface of GaAs. Compared with samples without etching, the diffraction efficiency can be significantly enhanced for samples with dry etching, due to the improvement of surface quality.