Bone‐Inspired Recyclable Composites for Damage‐Tolerant Circular Materials

Biological materials achieve remarkable combinations of mechanical performance and functionality through hierarchical architectures assembled across multiple length scales. Translating these principles into recyclable fiber‐reinforced composites remains challenging, as architecture‐enabled damage tolerance and circular material use are rarely integrated within a single design framework. Here, we report a recyclable bone‐inspired architected composite in which osteon‐like structures are assembled within an Elium thermoplastic acrylic matrix to enhance energy absorption, preserve a favorable strength‐toughness balance, and enable material recovery. Mimicking the crack‐arresting role of osteons, the embedded architecture redirects crack propagation and promotes energy dissipation, leading to a 95% increase in toughness modulus and 35% increase in strength under tensile loading compared to conventional laminates, while reduced transversal flexural performance highlights the loading‐direction‐dependent response of the discrete bone‐inspired architecture. Finite element simulations reproduce the force–displacement response and crack propagation patterns, revealing the mechanisms underlying damage tolerance. After matrix dissolution and component separation, the recovered osteon‐like structures retain tensile properties comparable to virgin counterparts. The modular architecture enables recovery of intact, aligned, load‐bearing units suitable for direct reuse without reprocessing or realignment. This work establishes a unified design and assembly strategy for recyclable bio‐inspired architected composites with coupled structural performance and circular functionality.