Harmonic structured materials with fine and coarse grains demonstrate not only enhanced strength but also enough ductility simultaneously. The harmonic structured material consists of a network like a fine grain region and a dispersed coarse grain region. The high strength and enough ductility are attributed to the network fine grain region and the dispersed coarse grain region, respectively. In this study, the harmonic structured metallic composite with high speed steel (HSS) and low carbon steel (LCS) is fabricated by mechanical milling and spark plasma sintering process. The harmonic structured HSS/LCS composite consists of the network like fine grain region with HSS and dispersed coarse grain region with LCS. The hardness of the harmonic structured composite with HSS and LCS is higher than the conventional particle dispersed composite with the same HSS volume fraction.Furthermore, the harmonic structured composite with HSS and LCS indicates high tensile strength without ductility loss, compared to the conventional HSS particle dispersed composite with the same HSS volume fraction. The harmonic structure control of composite materials is effective to improve the mechanical properties with enough ductility maintained.