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It is a challenge to synthesize high-quality MAPbX3 single-crystal microwires (MWs) under gentle conditions owing to their sensitivity to humidity and brittleness. We herein propose a facile bilayer flexible polymer confinement method to obtain high-quality MAPbI3 single-crystal microwires in air. The MAPbI3 microwire-based photodetector exhibits a superior responsivity of 77.96 A W−1, an EQE of 1.86 × 104%, and an ultrahigh detectivity of 6.97 × 1013 Jones owing to the efficient carrier transport and excellent crystallinity with few defects. Furthermore, photodetectors based on the MAPbI3 microwire arrays present superior performance with a detectivity of 3.09 × 1013 Jones, which is more than 160% and 7700% higher than that of the photodetectors based on the MAPbI3 microwires and polycrystalline film at 254 μW cm−2. [ABSTRACT FROM AUTHOR]