Electrodeposited amorphous alloys require numerous nuclei and irregular atomic arrangements. In this study, the impact of processing parameters (e.g., a nanosecond laser) on the current density in the electroplating solution for an electrodeposited NiP coating was tested using an electrochemical workstation. In addition, the effect of the laser on the temperature and micro-stirring caused by cavitation was simulated using COMSOL (version 5.4). The surface quality, wear, and corrosion resistance of the NiP coating prepared by laser-assisted electrodeposition (LECD) at different laser repetition frequencies (picosecond laser, 0.5, 1, 1.5, 2, and 2.5 MHz) were evaluated. The results showed that the stability of current change was best when the laser frequency, pulse width, scanning line spacing, and irradiation area were 1 MHz, 200 ns, 20 μm, 1 mm2, respectively. Excessive laser energy destroys the balance of electrochemical deposition process. The simulation results showed that the maximum instantaneous temperature of the laser-irradiated solution was 123 °C. Cavitation increases the flow rate of the solution and produces a jet impact on the substrate. The maximum velocity and instantaneous pressure were 0.13 m/s and 7.26 × 108 Pa at 0.1 ns, respectively. At the laser frequency of 0.5 MHz, the P content increases by approximately 2% compared to that of the coating prepared by LECD (1–2.5 MHz). The residual internal stress decreased with increasing frequency, and it existed in the form of tensile stress. The wear and corrosion resistances of the NiP coating were the best when the laser frequency was 1 MHz. Display omitted •Laser irradiation increases the current density of ECD.•Laser irradiation has a force impact on the solution.•Cavitation accelerates the flow velocity of solution and form jet impact.•Laser frequency affects the quality of electrodeposited layer.