Since the sound absorption mechanism of cylindrical-hole layer at low-frequency and at high-frequency are different, an optimization and design method for the sound absorption layer based on the multi-objective genetic algorithm was developed. First, the calculation procedure of the plane wave normally impinging on the sound absorption layer was modeled by using the ANSYS software. Next, the non-dominated sorting genetic algorithm II (NSGA-II) was adopted to solve this optimization problem and get the Pareto optimization. The results indicate that the coupled relationship between the low-frequency and the high-frequency can be both considered during the multi-objective optimization process, and designers can choose the satisfactory optimization results according to their demands. Besides, compared to the optimization of the material properties only, the simultaneous optimization of material properties and structural parameters may result in a higher sound absorption coefficient in a wider frequency range.