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The rational design of desirable lightweight structural materials usually needs to meet the strict requirements of mechanical properties. Seeking optimal integration strategies for lightweight structures and high mechanical performance is always of great research significance in the rapidly developing composites field, which also draws significant attention from materials scientists and engineers. However, the intrinsic incompatibility of low mass and high strength is still an open challenge for achieving satisfied engineering composites. Fortunately, creatures in nature tend to possess excellent lightweight properties and mechanical performance to improve their survival ability. Thus, by ingenious structure configuration, lightweight structural biomaterials with simple components can achieve high mechanical performance. This review comprehensively summarizes recent advances in three typical structures in natural biomaterials: cellular structures, fibrous structures, and sandwich structures. For each structure, typical organisms are selected for comparison, and their compositions, structures, and properties are discussed in detail, respectively. In addition, bioinspired design approaches of each structure are briefly introduced. At last, the outlook on the design and fabrication of bioinspired composites is also presented to guide the development of advanced composites in future practical engineering applications.