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Bi_1−xNd_xFe_0.99Mn_0.01O₃ (BNFMO, x = 0.00~0.20) films were epitaxially grown on Nb:SrTiO₃ (001) substrates using pulsed laser deposition. It was found that the Nd-doping concentration has a great impact on the surface morphology, crystal structure, and electrical properties. BNFMO thin film with low Nd-doping concentration (≤16%) crystallizes into a rhombohedral structure, while the high Nd-doping (>16%) will lead to the formation of an orthogonal structure. Furthermore, to eliminate the resistive switching (RS) effect, a positive-up–negative-down (PUND) measurement was applied on two devices in series. The remnant polarization experiences an increase with the Nd-doping concentration increasing to 16%, then drops down with the further increased concentration of Nd. Finally, the ferroelectric photovoltaic effect is also regulated by the ferroelectric polarization, and the maximum photocurrent of 1758 μA/cm² was obtained in Bi_0.84Nd_0.16Fe_0.99Mn_0.01O₃ thin film. BNFMO films show great potential for ferroelectric and photovoltaic applications.