Thermally activated blue-to-purple luminescence of Co-modified nano-sandrose MgAl-layered double hydroxides (LDHs) is concentration dependent, occurring only for MgCoAl-LDH with a molar metal cation concentration of 15% Co. Temperature sweep luminescence spectroscopy between 83 K and 298 K shows that the luminescence is strongest at room temperature, increasing with an activation energy of 1 kJ mol-1 between these temperatures. The luminescence occurs in a broad, but fine-structured band below the conduction band (CB) edge at 3.0 eV after excitation at 5.0 eV.