Among metal disilicide materials, α‐MoSi2 exhibits high thermal conductivity and high oxidation resistance at high temperatures, making it an attractive option for high temperature applications. In the present study, we fabricate α‐MoSi2 pellets with a density of 96% theoretical density (TD) and quantify the thermal properties (thermal conductivity and thermal expansion heat capacity), mechanical properties (Vickers hardness and fracture toughness), and electrical properties (Seebeck coefficient and electrical resistivity). In this paper, we evaluate the experimental data, and present a review of the literature. In addition, we attempt to correlate the heat capacity measurement obtained experimentally with the results of our theoretical calculations to identify their relationship.