Indoor photovoltaics (IPVs) have attracted increasing attention for sustainably powering Internet of Things (IoT) electronics. Sb₂S₃ is a promising IPV candidate material with a bandgap of ~1.75 eV, which is near the optimal value for indoor energy harvesting. However, the performance of Sb₂S₃ solar cells is limited by nonradiative recombination, which is dependent on the quality of the absorber films. Additive engineering is an effective strategy to fine tune the properties of solution-processed films. This work shows that the addition of monoethanolamine (MEA) into the precursor solution allows the nucleation and growth of Sb₂S₃ films to be controlled, enabling the deposition of high-quality Sb₂S₃ absorbers with reduced grain boundary density, optimized band positions, and increased carrier concentration. Complemented with computations, it is revealed that the incorporation of MEA leads to a more efficient and energetically favorable deposition for enhanced heterogeneous nucleation on the substrate, which increases the grain size and accelerates the deposition rate of Sb₂S₃ films. Due to suppressed carrier recombination and improved charge-carrier transport in Sb₂S₃ absorber films, the MEA-modulated Sb₂S₃ solar cell yields a power conversion efficiency (PCE) of 7.22% under AM1.5 G illumination, and an IPV PCE of 17.55% under 1000 lux white light emitting diode (WLED) illumination, which is the highest yet reported for Sb₂S₃ IPVs. Furthermore, we construct high performance large-area Sb₂S₃ IPV minimodules to power IoT wireless sensors, and realize the long-term continuous recording of environmental parameters under WLED illumination in an office. This work highlights the great prospect of Sb₂S₃ photovoltaics for indoor energy harvesting.

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