Proposed are a method of preparing new biomaterials for dental pulp regeneration and a composition of new biomaterials prepared accordingly. The composition of new biomaterials prepared according to the method of preparing new biomaterials for dental pulp regeneration by mixing a first precursor containing calcium silicate-based cement (CSC) at an appropriate concentration and a second precursor containing a secretome of dental pulp-derived mesenchymal stem cells in an appropriate ratio and then drying the resulting mixture under appropriate drying conditions is characterized by further improving the osteogenic differentiation ability of dental pulp stem cells compared to existing materials while maintaining the microhardness of the composition to an appropriate standard. In addition, the composition is advantageous in that an aesthetic effect is excellent by not causing tooth discoloration.