High Mechanical Strength Alloy‐like Minerals Prepared by Inorganic Ionic Co‐cross‐linking

Abstract Alloys often combine different metals to generate superior mechanical properties. However, it is challenging to prepare high mechanical strength minerals with similar strategies. Using calcium carbonate (CaC) and calcium phosphate (CaP) as examples, this work synthesizes a group of compounds with the chemical formulas Ca(CO 3 ) x (PO 4 ) 2(1‐ x )/3 (0 < x < 1, CaCPs) by cross‐linking ionic oligomers. Unlike mixtures, these CaCPs exhibit a single temperature for the phase transition from amorphous to crystallized CaC (calcite) and CaP (hydroxyapatite). By heat‐induced synchronous crystallization, dual‐phase CaC/CaP with continuous crystallized boundaries are resembled to alloy‐like minerals (ALMs). The mechanical properties of the ALMs are adjusted by tailoring their chemical compositions to reach a hardness of 5.6 GPa, which exceed those of control calcite and hydroxyapatite samples by 430% and 260%, respectively. This strategy expands the chemical scope of inorganic materials and holds promise for preparing high‐performance minerals.