α-SiAlON is commonly used to machine superalloys owing to its desirable thermal and structural properties. α-SiAlON is among the crystalline forms of SiAlON and has more favorable properties than β-SiAlON. However, it becomes fragile during the machining of hard-to-cut materials due to its low fracture toughness and machinability. Recent research efforts focus on improving the thermal and structural properties of α-SiAlON using suitable dopants, nano-sized precursors, and the addition of metallic/ceramic reinforcement particles. The present study presents a material-by-design approach to designing and developing ceramic and metal-particle-reinforced Ca-α-SiAlON composites with properties tailored for the cutting tool applications. The mean-field homogenization theories and effective medium approximations implemented in an in-house code are used to effectively optimize the thermal and structural properties of the Ca-α-SiAlON composite by varying essential parameters such as inclusion material, volume fraction, porosity, particulate size, and thermal interface resistance. Individual properties of the matrix and reinforcements are considered in the computations of effective properties such as thermal conductivity, thermal expansion coefficient, modulus of elasticity, and fracture toughness. The main objective of the study is to enhance the thermal conductivity and fracture toughness of Ca-α-SiAlON, while lowering its thermal expansion coefficient. At the same time, the elastic modulus and hardness/strength must be maintained within an acceptable range. As a validation, Ni/Ca-α-SiAlON and SiC/Ca-α-SiAlON composites are synthesized from the nano-sized precursors, CaO dopant, and Ni/SiC microparticles via spark plasma sintering (SPS) process. The thermal conductivity, coefficient of thermal expansion, and elastic modulus of the composites are measured and compared with the computational predictions. The computational predictions are found to be comparable to that of the experimental measurements. Moreover, the studies show that WC, SiC, and Cr can be suitable reinforcement materials for enhancing the thermal and structural properties of Ca-α-SiAlON material for the cutting tool inserts.