ABSTRACT Ceramics are stiff and thermally stable but dissipate little fracture energy, often failing catastrophically. Introducing soft interlayers can increase toughness, yet they frequently compromise high‐temperature integrity, creating an interfacial dilemma between dissipation and cohesion. Here, we show that fracture in dense, all‐ceramic nacre‐like microstructures can be programmed through designed interfacial mineral nanobridges. We derive a crack‐deflection criterion that links interface–microplatelet toughness contrast to nanobridge connectivity and dimensions, yielding a design map in nanobridge coverage and width that predicts when cracks deflect along interfaces versus penetrate microplatelets. Discrete‐element simulations reproduce the transition and identify an optimal mixed‐mode regime that maximizes dissipation while preserving microplatelet load bearing. Utilizing it, we fabricate polymer‐free nacre‐like alumina–zirconia microstructures with tunable zirconia nanobridges by magnetically assisted assembly and controlled sintering. Optimized interfaces deliver an unusual property combination: fracture toughness ∼13.9 MPa·m 0.5 , flexural strength >347 MPa, and damping ( tan δ ≈ 0.031), with frequency stability (1–100 Hz), temperature stability till 500°C, and thermomechanical dimensional stability up to 1300°C. When shaped into a tooth‐like construct, the material reproduces enamel–dentin anisotropy and graded organization while maintaining hydrothermal phase stability and cytocompatibility. This interface design strategy provides a platform for tough, stable, bioinspired all‐ceramic materials for versatile applications.
Behera et al. (2026) studied this question.