The high-quality ZnO films are deposited on glass and silicon substrates using a laser deposition process in different burst modes, with the number of subpulses in each burst increasing from 1 to 4. The effects of different burst modes of picosecond lasers on the film thickness, roughness, surface topography, crystal structure, optical properties, and electrical properties of ZnO films are investigated. When the pulse burst mode is set to 4, the film surface has less roughness, smaller particle size, higher transmittance, better crystalline quality, and lower resistivity when compared with other burst modes. This is extremely important for relevant optical applications to the production of ZnO thin film.