The remarkable damage-tolerance found in natural materials is developed through functional, multiscale architectures with structural gradients and graded interfaces. [1][2][3][4][5][6] One notable example is nacre, which comprises ceramic (mineral) platelets of polycrystalline aragonite (≈95% by volume) bonded by biopolymers in a "brick-and-mortar" structure. [1,3,7] The Many natural materials present an ideal "recipe" for the development of future damage-tolerant lightweight structural materials. One notable example is the brick-and-mortar structure of nacre, found in mollusk shells, which produces high-toughness, bioinspired ceramics using polymeric mortars as a compliant phase. Theoretical modeling has predicted that use of metallic mortars could lead to even higher damage-tolerance in these materials, although it is difficult to melt-infiltrate metals into ceramic scaffolds as they cannot readily wet ceramics. To avoid this problem, an alternative ("bottomup") approach to synthesize "nacre-like" ceramics containing a small fraction of nickel mortar is developed. These materials are fabricated using nickelcoated alumina platelets that are aligned using slip-casting and rapidly sintered using spark-plasma sintering. Dewetting of the nickel mortar during sintering is prevented by using NiO-coated as well as Ni-coated platelets. As a result, a "nacre-like" alumina ceramic displaying a resistance-curve toughness up to ≈16 MPa m ½ with a flexural strength of ≈300 MPa is produced. Ceramic-Metal Composites www.advancedsciencenews.com