Biomimetic Mechanical Robust Cement‐Resin Composites with Machine Learning‐Assisted Gradient Hierarchical Structures

Abstract Biological materials relying on hierarchically ordered architectures inspire the emergence of advanced composites with mutually exclusive mechanical properties, but the efficient topology optimization and large‐scale manufacturing remain challenging. Herein, this work proposes a scalable bottom‐up approach to fabricate a novel nacre‐like cement‐resin composite with gradient brick‐and‐mortar (BM) structure, and demonstrates a machine learning‐assisted method to optimize the gradient structure. The fabricated gradient composite exhibits an extraordinary combination of high flexural strength, toughness, and impact resistance. Particularly, the toughness and impact resistance of such composite attractively surpass the cement counterparts by factors of approximately 700 and 600 times, and even outperform natural rocks, fiber‐reinforced cement‐based materials and even some alloys. The strengthening and toughening mechanisms are clarified as the regional‐matrix densifying and crack‐tip shielding effects caused by the gradient BM structure. The developed gradient composite not only endows a promising structural material for protective applications in harsh scenarios, but also paves a new way for biomimetic metamaterials designing.