Amplification in toughness and balance with stiffness and strength are fundamental characteristics of biological structural composites, and a long sought-after objective for engineering design. Nature achieves these properties through a combination of multiscale key features. Yet, emulating all these features into synthetic de novo materials is rather challenging. Here, we fine-tune manual lamination, to implement a newly designed bone-inspired structure into fiber-reinforced composites. An integrated approach, combining numerical simulations, ad hoc manufacturing techniques, and testing, yields a novel composite with enhanced fracture toughness and balance with stiffness and strength, offering an optimal lightweight material solution with better performance than conventional materials such as metals and alloys. The results also show how the new design significantly boosts the fracture toughness compared to a classic laminated composite, made of the same building blocks, also offering an optimal tradeoff with stiffness and strength. The predominant mechanism, responsible for the enhancement of fracture toughness in the new material, is the continuous deviation of the crack from a straight path, promoting large energy dissipation and preventing a catastrophic failure. The new insights resulting from this study can guide the design of de novo fiber-reinforced composites toward better mechanical performance to reach the level of synergy of their natural counterparts.