This paper tries to investigate a novel polishing technology with high efficiency and nice surface quality for sapphire crystal that has high hardness, wear resistance, and chemical stability. A Q-switched 355 nm ultraviolet laser with nanosecond pulses was set up and used to polish sapphire substrate in different conditions in this paper. Surface roughness Ra of polished sapphire was measured with surface profiler, and the surface topography was observed with scanning electronic microscope. The effects of processing parameters as laser energy, pulse repetition rate, scanning speed, incident angle, scanning patterns, and initial surface conditions on surface roughness were analyzed.