Nature has developed a wide range of functional microstructures with optimized mechanical properties over millions of years of evolution. By learning from nature’s excellent models and principles, biomimicry provides a practicable strategy for designing and fabricating the next smart materials with enhanced properties. Nevertheless, the complicated micro-structural constructions in nature models are beyond the ability of conventional processes, hindering the developments of biomimetic research and its forthputting in engineering systems. Additive manufacturing (AM) or 3D printing processes have revolutionized manufacturing via their ability to manufacture complex micro/mesostructures, increase design freedom, provide mass customization, and waste minimization, as well as rapid prototyping. Here, a review of recent advances in biomimetic 3D printing materials with enhanced mechanical properties is provided. The design and fabrication were inspired by various natural structures, such as balsa wood, honeycomb, nacre, lobster claw, etc., which are presented and discussed. Finally, future challenges and perspectives are given.