Enhancement of the perovskite film quality and charge transfer capability is crucial for enhancing device performance. The all-inorganic CsPbCl3 perovskite, which shows great potential as an absorber layer in ultraviolet photodetectors (UV PDs), has been hindered by poor material stability and high interface states, limiting its widespread application. In this work, the quality of the CsPbCl3 films and the perovskite/Au electrode interface were synergistically modulated using V2CTx MXene. After additive (CsPbCl3@V2CTx) and interface (CsPbCl3/V2CTx) engineering, the optimal properties of CsPbCl3 films and the van der Waals (vdW) bonding of V2CTx strengthen the charge extraction and hole transport while reducing nonradiative charge recombination caused by internal defects and interface states. Ultimately, the UV PD featuring the FTO/SnO2/CsPbCl3@V2CTx/V2CTx/Au structure manifests outstanding performance under the self-powered mode, attaining an extremely high responsivity of up to 1.01 × 103 mA/W and a considerable specific detectivity of 5.46 × 1011 cm Hz1/2/W (365 nm, 0.16 mW/cm2) coupled with a swift rise/decay time of 1.54/1.50 μs. Even after 30 days under an air atmosphere, the responsivity of the device remains at 8.46 × 102 mA/W, indicating extraordinary stability. This approach offers a novel way to enhance the performance of UV PD based on the CsPbCl3 perovskite through the dual strategy of V2CTx MXene modulation.