In the quest of increasing safety and efficiency in structural applications, by designing and manufacturing new strong and tough composite materials, learning from the design of natural materials can be a promising strategy. Nature has evolved for billions of years to develop elaborate architectures and sophisticated strategies, based on mechano-biological mechanisms, to achieve optimally adapted material solutions. A brief review of exemplar naturally occurring materials is provided, here, with a focus on their multiscale structures and the mechanisms governing their mechanical properties. The design motifs, common to biological structural materials, and the mechanisms underlying their characteristics are summarized, with a highlight on the structureproperty relationship. A review of recent advancement in the manufacturing of bio-inspired composite materials, mainly inspired by bone, nacre, and teeth, is provided, followed by recent and successful case studies. In this paper, the main focus is on nacre and bone-inspired structural materials, aimed at mimicking the mechanical behavior. Finally, a critical discussion is provided, highlighting the limitations of the current innovative techniques and materials, and prospecting the future challenges for the design and development of de novo materials and manufacturing processes for real engineering applications.