The process parameters of LLDPE/EVA/nano-ZnO composites were optimized by two methods. Samples were prepared under the better process parameters. The dispersion morphology and the mechanical properties of material were studied by Field Emission Scanning Electron Microscope (FESEM). And the mechanical properties of LLDPE/EVA/nano-ZnO composites were tested. It was showed that the optimization method based on neural network of BP and particle swarm optimization was better than that optimization method based on orthogonal experiment. The nanoeffect of ZnO particles was exerted which were distributed in LLDPE/EVA matrix, which result in the effect of reinforcing and toughening. Two-step method was better than direct dispersing method. The tensile strength was the highest when nano-ZnO amount was 3% under the two-step, the tensile strength was increased up to about 22%, and the fracture elongation rate was increased up to about 11%.