Perovskite light-emitting diodes (PeLEDs) have gained significant attention owing to their remarkable tunability and color stability, and substantial progress has been made with green and red PeLEDs. However, the advancement of blue PeLEDs still lags far behind their red and green counterparts. In this study, we report efficient sky-blue PeLEDs utilizing an in situ fabricated CsPb2Br5 plates/quasi-2D perovskite heterojunction using chelating molecules to modulate the crystallization process of perovskites. The wide bandgap of CsPb2Br5 facilitated the formation of a type-I band alignment at the heterojunction, allowing efficient carrier transfer from CsPb2Br5 to CsPbBr3. This heterojunction leads to a noteworthy enhancement of device efficiency. The PeLEDs exhibit a maximum brightness of 2311 cd m-2, accompanied by a maximum external quantum efficiency of 12.86% at 487 nm. Our tailored design of CsPb2Br5/perovskite heterojunction thin films offers a promising avenue for advancing PeLED performance. This work contributes valuable insights into the burgeoning field of perovskite electroluminescence, paving the way for further optimization of PeLED technologies.