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Organic–inorganic halide perovskites are promising photodetector materials due to their strong absorption, large carrier mobility, and easily tunable bandgap. Up to now, perovskite photodetectors are mainly based on polycrystalline thin films, which have some undesired properties such as large defective grain boundaries hindering the further improvement of the detector performance. Here, perovskite thin‐single‐crystal (TSC) photodetectors are fabricated with a vertical p–i–n structure. Due to the absence of grain‐boundaries, the trap densities of TSCs are 10–100 folds lower than that of polycrystalline thin films. The photodetectors based on CH₃NH₃PbBr₃and CH₃NH₃PbI₃TSCs show low noise of 1–2 fA Hz^−1/2, yielding a high specific detectivity of 1.5 × 10¹³cm Hz^1/2W⁻¹. The absence of grain boundaries reduces charge recombination and enables a linear response under strong light, superior to polycrystalline photodetectors. The CH₃NH₃PbBr₃photodetectors show a linear response to green light from 0.35 pW cm⁻²to 2.1 W cm⁻², corresponding to a linear dynamic range of 256 dB.

The surface composition of perovskite films is very sensitive to film processing and can deviate from the optimal, which generates unfavorable defects and results in efficiency loss in solar cells and slow response speed in photodetectors. An argon plasma treatment is introduced to modify the surface composition by tuning the ratio of organic and inorganic components as well as defect type before deposition of the passivating layer. It can efficiently enhance the charge collection across the perovskite–electrode interface by suppressing charge recombination. Therefore, perovskite solar cells with argon plasma treatment yield enhanced efficiency to 20.4% and perovskite photodetectors can reach their fastest respond speed, which is solely limited by the carrier mobility.