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The Cu2ZnSnS4 (CZTS) thin films were fabricated by sulfurization of radiofrequency magnetron sputtered Cu–Zn–Sn–O (CZTO) precursors. Here, we extend recent works in the field of fabricating CZTO precursors by a new approach sputtering ZnO/Sn/Cu targets. The effects of one-step and two-step annealing processes applied for CZTO precursors on the structure, morphology, optical, and electrical properties were investigated systematically. The preannealing step of fundamental phase formation in the sulfurization process was also discussed. The two-step annealing process was found to affect the composition of element Sn slightly but significantly improved crystallinity, CZTS/Mo interfacial conditions, surface roughness, and electrical properties. The two-step annealed CZTS thin films had excellent optical and electrical properties with an optical band gap of 1.51 eV, a hole concentration of 2.4 × 1017 cm−3, and a hole mobility of 1.97 cm2/(V⋅s). In addition, the CZTS/Mo interface with small grains and voids were significantly improved. CZTS-based solar cell devices were successfully fabricated. The characteristics of current–voltage (J–V) curves indicated that short-circuit currents had a tendency to increase with the improvement of CZTS/Mo interface and surface morphology. As a result, the device based on two-step annealed CZTS thin films exhibited better performance with an open-circuit voltage of 553 mV, short-circuit current of 7.2 mA⋅cm−2, a fill factor of 37.8%, and a conversion efficiency of 1.51%.