Polyurethane (PU) foams are widely used as acoustic package materials to eliminate vehicle interior noise. Therefore, it is important to improve the acoustic performances of PU foams. In this paper, the grey relational analysis (GRA) method and multi-objective particle swarm optimization (MOPSO) algorithm are applied to improve the acoustic performances of PU foam composites. The average sound absorption coefficient and average transmission loss are set as optimization objectives. The hardness and content of Ethylene Propylene Diene Monomer (EPDM) and the content of deionized water and modified isocyanate (MDI) are selected as design variables. The optimization process of GRA method is based on the orthogonal arrays , and the MOPSO algorithm is based on the Response Surface (RS) surrogate model. The results show that the acoustic performances of PU foam composites can be improved by optimizing the synthetic formula. Meanwhile, the results that were obtained by GRA method show the degree of influence of the four design variables on the optimization objectives, and the results obtained by MOPSO algorithm show the specific effects of the four design variables on the optimization objectives. Moreover, according to the confirmation experiment, the optimal synthetic formula is obtained by MOPSO algorithm when the weight coefficient of the two objectives set as 0.5.