The improvement of the thermoelectric performance of semiconducting chalcogenides is an important task. The principal challenge in this field is to tailor the thermoelectric properties, such as electrical conductivity, Seebeck coefficient, and thermal conductivity, to improve the figure of merit (ZT). Herein, we present an improvement in the thermoelectric properties of InIII‐doped p‐type Cu3SbSe4 thin films deposited by using a microwave‐assisted technique. The deposited thin films were characterized for their optical, structural, morphological, compositional, and electrical transport properties to show the applicability of the materials in thermoelectric energy conversion. The improvement in ZT is achieved with InIII doping because of the enhancement in the charge carrier density of Cu3SbSe4 thin films. A maximum ZT of 0.183 was achieved for Cu3(Sb0.94In0.06)Se4 at 300 K. Our results show that this deposition strategy and doping process can provide an effective solution to fabricate Cu3SbSe4‐based materials for thermoelectric applications.