To address the issue of local optima encountered during the multi-objective optimization process with the Non-dominated Sorting Genetic Algorithm II (NSGA-II) algorithm, this paper introduces an enhanced version of the NSGA-II. This improved NSGA-II incorporates polynomial and simulated binary crossover operators into the genetic algorithm’s crossover phase to refine its performance. For evaluation purposes, the classic ZDT benchmark functions are employed. The findings reveal that the enhanced NSGA-II algorithm achieves higher convergence accuracy and surpasses the performance of the original NSGA-II algorithm. When applied to the machining of the high-hardness material 20MnCrTi, four algorithms were utilized: the improved NSGA-II, the conventional NSGA-II, NSGA-III, and MOEA/D. The experimental outcomes show that the improved NSGA-II algorithm delivers a more optimal combination of process parameters, effectively enhancing the workpiece’s surface roughness and material removal rate. This leads to a significant improvement in the machining quality of the workpiece surface, demonstrating the superiority of the improved algorithm in optimizing machining processes.