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A smelting multiple recrystallization strategy and its effects on the morphology, composition, and defects of CsPbBrI2 film were investigated. An optimal number (n = 2) of recrystallization cycles improved the crystallinity and phase purity, minimized the grain boundaries, and optimized the crystal structure, yielding a high-quality perovskite film with significantly reduced defects density. The corresponding photovoltaic devices exhibited a champion efficiency of 16.02% under AM 1.5 G illumination and presented an even higher indoor efficiency of 33.50% under an LED (2956 K, Pin: 334.41 μW/cm2). This recrystallization method offers a promising strategy for developing high-performance indoor and outdoor photovoltaics. Direct recrystallization in the cells was also explored to achieve enhanced stability and longer lifetime in humid conditions.