The self-excited oscillation pulsed atomizing nozzle can effectively and evenly spray the high-speed solid cone jet without any extra power. The primary atomization of the jet at the outlet of nozzle directly affects the final spray quality, and the turbulence and cavitation at the outlet of the atomizing nozzle are the other two main factors affecting the atomization. In this work, multi-objective optimization depending on nozzle parameters was established by using mathematical optimization techniques and computational fluid dynamics to improve the jet atomization quality at the outlet of the nozzle. The central composite design method and the response surface method were used to obtain the approximate mathematical model of the primary atomization quality of the jet at the outlet of nozzle. Finally, the non-dominated sorting genetic algorithm with elitist strategy (NSGA-II) and the grey theory were used in combination to optimize the nozzle parameters. Through combining with the NSGA-II and the grey theory, the nozzle parameters were optimized in order to obtain the best primary atomization at the outlet area of nozzle. The optimization results verified the nozzle design with multi-objective optimization method. The optimized values of the turbulent kinetic energy F 1 and the vapor volume fraction F 2 increased by 28.26% and 5.56%, respectively, and the corresponding nozzle parameters of the chamber diameter D, the lower nozzle diameter d 2 and the upper nozzle inlet pressure P in were, respectively, optimized to 28.056 mm, 5.472 mm and 3.999 Mpa.