jats:titleAbstract</jats:title>jats:pWith the exponential rise in the market value and number of devices part of the Internet of Things (IoT), the demand for indoor photovoltaics (IPV) to power autonomous devices is predicted to rapidly increase. Lead‐free perovskite‐inspired materials (PIMs) have recently attracted significant attention in photovoltaics research, due to the similarity of their electronic structure to high‐performance lead‐halide perovskites, but without the same toxicity limitations. However, the capability of PIMs for indoor light harvesting has not yet been considered. Herein, two exemplar PIMs, BiOI and Csjats:sub3</jats:sub>Sbjats:sub2</jats:sub>Cljats:italicjats:subx</jats:sub></jats:italic>Ijats:sub9‐</jats:sub>jats:italicjats:subx</jats:sub></jats:italic> are examined. It is shown that while their bandgaps are too wide for single‐junction solar cells, they are close to the optimum for indoor light harvesting. As a result, while BiOI and Csjats:sub3</jats:sub>Sbjats:sub2</jats:sub>Cljats:italicjats:subx</jats:sub></jats:italic>Ijats:sub9‐</jats:sub>jats:italicjats:subx</jats:sub></jats:italic> devices are only circa 1%‐efficient under 1‐sun illumination, their efficiencies increase to 4–5% under indoor illumination. These efficiencies are within the range of reported values for hydrogenated amorphous silicon, i.e., the industry standard for IPV. It is demonstrated that such performance levels are already sufficient for millimeter‐scale PIM devices to power thin‐film‐transistor circuits. Intensity‐dependent and optical loss analyses show that future improvements in efficiency are possible. Furthermore, calculations of the optically limited efficiency of these and other low‐toxicity PIMs reveal their considerable potential for IPV, thus encouraging future efforts for their exploration for powering IoT devices.</jats:p>