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The notion of replicating the unique fracture resistance of natural composites in synthetic materials has generated much interest but has yielded few real technological advances. Here we demonstrate how using ice-templated structures, the concept of hierarchical design can be applied to conventional compounds such as alumina and poly(methyl methacrylate) (PMMA) to make bulk hybrid materials that display exceptional toughness that can be nearly 300 times higher (in energy terms) than either of their constituents. These toughnesses far surpass what can be expected from a simple “rule of mixtures”; for a ∼80% Al₂O₃–PMMA material, we achieve a K_Jc fracture toughness above 30MPam^1/2 at a tensile strength of ∼200MPa. Indeed, in terms of specific strength and toughness, these properties for alumina-based ceramics are at best comparable to those of metallic aluminum alloys. The approach is flexible and …