Abstract The study of acoustic metamaterials, also known as locally resonant sonic materials, has recently focused on the topic of underwater sound absorption. The high absorption occurs only within a narrow frequency band around the locally resonant frequency. Nevertheless, this problem can be addressed through a combination of several acoustic metamaterial layers that have different resonant frequencies. In this paper, an optimization scheme, a genetic and a general nonlinear constrained algorithm, is utilized to enhance the low-frequency underwater sound absorption of an acoustic metamaterial slab with several layers. Both the physical and structural parameters of the acoustic metamaterial slab are optimized to enlarge the absorption band. In addition, the sound absorption mechanism of the acoustic metamaterial slab is also analyzed. The result shows that each layer is found to oscillate as a nearly independent unit at its corresponding resonant frequency. The theoretical and experimental results both demonstrate that the optimized metamaterial slab can achieve a broadband (800–2500 Hz) absorption of underwater sound, which is a helpful guidance on the design of anechoic coatings.