Composites, materials composed of two or more materials—metallic, organic, or inorganic—usually exhibit the combined physical properties of their component materials. The result is a material that is superior to conventional monolithic materials. Advanced composites are used in a variety of industrial applications and therefore attract much scientific interest. Here the formation of novel carbon‐based nanocomposites is described via incorporation of graphene oxide (GO) into the crystal lattice of single crystals of calcite. Incorporation of a 2D organic material into single‐crystal lattices has never before been reported. To characterize the resulting nanocomposites, high‐resolution synchrotron powder X‐ray diffraction, electron microscopy, transmission electron microscopy, fluorescence microscopy and nanoindentation tests are employed. A detailed analysis reveals a layered distribution of GO sheets incorporated …