In the quest for new materials, we introduce self-consistent ab initio simulations to investigate the structural and mechanical stability, electronic profile, and transport properties of f-electron-based RaMO3 (M = Cm, Bk) perovskites by employing density functional theory. The energy optimization indicates that these alloys exhibit stability in the ferromagnetic phase. The examination of mechanical parameters demonstrates the ductile nature of these materials. To elucidate the electronic structure of these alloys, we employed a combination of two approximations: Generalized Gradient Approximation (GGA) and GGA + mBJ. Both approximations confirm the alloys’ half-metallic character. The magnetic moments calculated using both approximations were approximately 6 µB for RaCmO3 and approximately 7 µB for RaBkO3. The thermoelectric performance of these materials is evaluated by investigating different transport parameters such as the Seebeck coefficient, electrical and thermal conductivity and power factor. The comprehensive investigation of these two alloys has the potential to expand their applications in spintronics, thermoelectric devices, and radioisotope thermoelectric generators (RTGs).