All‐inorganic CsPbCl3 perovskite has emerged as a promising material for ultraviolet (UV) photodetection, attributed to its appropriate bandgap and exceptional optoelectronic properties. However, the suboptimal film‐forming quality of the solution process, as well as the instability of films induced by UV radiation and the annealing process, have limited its popularization and application. Herein, the buried layer is pretreated with N, N‐dimethylacetamide (DMF) to improve surface hydrophilicity and facilitate the anchoring of Pb2+. Additionally, Nb2CTx is incorporated into the PbCl2 precursor solution to enhance the quality of CsPbCl3 films. Following surface engineering and Nb2CTx modification (CsPbCl3@Nb2CTx), the morphology and optoelectronic properties of CsPbCl3 films are optimized. Furthermore, the effect of lattice strain and defect state‐induced interface state on the nonradiative charge recombination is mitigated. Ultimately, the UV photodetector fabricated on fluorine‐doped tin oxide (FTO)/SnO2/CsPbCl3@Nb2CTx/Au architecture exhibits outstanding performance including remarkably high responsivity (up to 990 mA W−1), significant specific detectivity (1.03 × 1011 cm Hz1/2 W−1), and rapid rise/decay time (0.24/0.32 µs) under self‐powered mode, with markedly improved stability as well. This approach presents a novel strategy for optimizing CsPbCl3 films through MXene modulation as an immense potential absorb layer for UV photodetector.