We report intriguing characteristics of light-induced and tunable shift currents in $\mathrm{B}{\mathrm{i}}_{1-\mathrm{x}}\mathrm{S}{\mathrm{m}}_{\mathrm{x}}\mathrm{Fe}{\mathrm{O}}_3\left(0.00\le \mathrm{x}\le 0.18\right)$ films, reflecting contributions from optoelectronic processes through structural phase evolution. Optical reflectance spectroscopy reveals asymmetry in sub-band-gap and direct-band-gap transitions, indicating phase-induced energy-level shifts. We demonstrate how visible light dramatically alters transitions involving $\mathrm{O}\text{−}2p\leftrightarrow \mathrm{Fe}-3d$ exchange interactions, and how continuous-wave illumination selectively excites charge carriers in ${\mathrm{Bi}}_{1-x}{\mathrm{Sm}}_x{\mathrm{FeO}}_3$, leading to spatial separation into localized and bandlike states upon optical transitions, thereby laying out all spatial control routes to shift photovoltaic currents.

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• Doping effects
• Electronic structure
• Optoelectronics
• Phase separation
• Photocurrent
• Photoinduced effect
• Polarons
• Quantum transport
• Structural properties
• Film deposition