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This study reports on substantial improvement of the open‐circuit voltage (V_oc) of Cu₂ZnSnSe₄ (CZTSe) thin film solar cells by applying a passivation strategy to both the top and bottom interfaces of the CZTSe absorber, which involves insertion of a thin dielectric layer between the CZTSe and the surrounding layers. The study also presents in‐depth material characterizations using transmission electron microscopy, energy dispersive X‐ray spectroscopy, low‐temperature photoluminescence, and secondary ion mass spectrometry, to reveal the effects of the interface passivation. To passivate the bottom Mo/CZTSe interface, a dielectric layer with patterned local contacts of dimensions down to ~100 nm was prepared using nanosphere lithography. With this, the V_oc, short‐circuit current, and fill factor (FF) were significantly enhanced due to reduction in carrier recombination at the bottom Mo/CZTSe interface. The …