The focus of this study is to investigate the effect of Al2O3 on α-calcium silicate (α-CaSiO3) ceramic. α-CaSiO3 was synthesized from CaO and SiO2 using mechanochemical method followed by calcinations at 1000°C. α-CaSiO3 and alumina were grinded using ball mill to create mixtures, containing 0-50w% of Al2O3 loadings. The powders were uniaxially pressed and followed by cold isostatic pressing (CIP) in order to achieve greater uniformity of compaction and to increase the shape capability. Afterward, the compaction was sintered in a resistive element furnace at both 1150°C and 1250°C with a 5h holding time. It was found that alumina reacted with α-CaSiO3 and formed alumina-rich calcium aluminates after sintering. An addition of 15wt% of Al2O3 powder at 1250°C were found to improve the hardness and fracture toughness of the calcium silicate. It was also observed that the average grain sizes of α-CaSiO3 /Al2O3 composite were maintained 500-700nm after sintering process.