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New solar cells with Ag/C60/MAPbI3/Cu2ZnSnSe4 (CZTSe)/Mo/FTO multilayered structures on glass substrates have been prepared and investigated in this study. The electron-transport layer, active photovoltaic layer, and hole-transport layer were made of C60, CH3NH3PbI3 (MAPbI3) perovskite, and CZTSe, respectively. The CZTSe hole-transport layers were deposited by magnetic sputtering, with the various thermal annealing temperatures at 300 °C, 400 °C, and 500 °C, and the film thickness was also varied at 50~300 nm The active photovoltaic MAPbI3 films were prepared using a two-step spin-coating method on the CZTSe hole-transport layers. It has been revealed that the crystalline structure and domain size of the MAPbI3 perovskite films could be substantially improved. Finally, n-type C60 was vacuum-evaporated to be the electronic transport layer. The 50 nm C60 thin film, in conjunction with 100 nm Ag electrode layer, provided adequate electron current transport in the multilayered structures. The solar cell current density–voltage characteristics were evaluated and compared with the thin-film microstructures. The photo-electronic power-conversion efficiency could be improved to 14.2% when the annealing temperature was 500 °C and the film thickness was 200 nm. The thin-film solar cell characteristics of open-circuit voltage, short-circuit current density, fill factor, series-resistance, and Pmax were found to be 1.07 V, 19.69 mA/cm2, 67.39%, 18.5 Ω and 1.42 mW, respectively.