Structural materials such as ceramics, metals, and carbon fiber-reinforced plastics (CFRP) are frequently threatened by large compressive and impact forces. Energy absorption layers, i.e., polyurethane and silicone foams with excellent damping properties, are applied on the surfaces of different substrates to absorb energy. However, the amount of energy dissipation and penetration resistance are limited in commercial polyurethane foams. Herein, a distinctive nacre-like architecture design strategy is proposed by integrating hard porous ceramic frameworks and flexible polyurethane buffers to improve energy absorption and impact resistance. Experimental investigations reveal the bioinspired designs exhibit optimized hardness, strength, and modulus compared to that of polyurethane. Due to the multiscale energy dissipation mechanisms, the resulting normalized absorbed energy (≈8.557MJ m-3) is ≈20 times higher than polyurethane foams under 50% quasi-static compression. The bioinspired composites provide superior protection for structural materials (CFRP, glass, and steel), surpassing polyurethane films under impact loadings. It is shown CFRP coated with the designed materials can withstand more than ten impact loadings (in energy of 10 J) without obvious damage, which otherwise delaminates after a single impact. This biomimetic design strategy holds the potential to offer valuable insights for the development of lightweight, energy-absorbent, and impact-resistant materials.