CsPbCl3 has gained enormous attention since its discovery and showed great potential in ultraviolet photodetectors over the past few years. Processing CsPbCl3 films through traditional solution methods hits a bottleneck due to their extremely poor precursor solubility. Here, high quality CsPbCl3 films were fabricated through vacuum thermal evaporation without the limitation of solubility. The structure of the evaporated CsPbCl3 films is a tetragonal phase with lattice constants different from those in common open source databases. The properties were thus first revealed by experimental characterization methods and theoretical calculations. Then, CsPbCl3 based photodetectors were constructed with evaporated pentacene films as a heterointerface layer to suppress severe charge recombination at the interfaces. The dark current of these photodetectors based on CsPbCl3–pentacene hybrid films decreases by more than two orders of magnitude, obtaining an enhanced on/off ratio, responsivity, and detectivity of 1.08 × 106, 248 mA W−1, and 2.04 × 1013 Jones with growth values of 34 000%, 35%, and 12 000%, respectively. These are benefitted greatly from the optimized surface morphology and carrier transport, which is evidenced by experiments and density functional theory (DFT) calculations. CsPbCl3 based photodetector arrays were further constructed, achieving character recording. The additional pentacene film in the devices showed an effect on image denoising. Our work provides a feasible method for constructing high performance ultraviolet photodetectors, enlightening the significance of material combination for other optoelectronic devices.