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Organic–inorganic halide perovskites are intrinsically unstable when exposed to moisture and/or light. Additionally, the presence of lead in many perovskites raises toxicity concerns. Herein, a thin film of barium zirconium sulfide (BaZrS₃), a lead‐free chalcogenide perovskite, is reported. Photoluminescence and X‐ray diffraction measurements show that BaZrS₃is far more stable than methylammonium lead iodide (MAPbI₃) in moist environments. Moisture‐ and light‐induced degradations in BaZrS₃and MAPbI₃are compared by using simulations and calculations based on density functional theory. The simulations reveal drastically slower degradation in BaZrS₃due to two factors—weak interaction with water and very low rates of ion migration. BaZrS₃photodetecting devices with photoresponsivity of ≈46.5 mA W⁻¹are also reported. The devices retain ≈60% of their initial photoresponse after 4 weeks under ambient conditions. Similar MAPbI₃devices degrade rapidly and show a ≈95% decrease in photoresponsivity in just 4 days. The findings establish the superior stability of BaZrS₃and strengthen the case for its use in optoelectronics. New possibilities for thermoelectric energy conversion using these materials are also demonstrated.