The quantum cutting ytterbium (Yb3+)-doped CsPbX3 (X = Cl, Cl, or Br) nanocrystals, exhibiting photoluminescence quantum yields (PLQYs) exceeding 100%, hold significant promise for applications in solar energy conversion technologies and near-infrared (NIR) light-emitting diodes (LEDs). This work investigates the usage of chlorophyll (CHL), a naturally existing organic pigment, as an efficient molecular passivator to improve the performance of quantum cutting films. With the assistance of CHL, the resultant perovskite film displays an increased PLQY of 176%. The commercial silicon solar cells (SSCs) with CHL-treated perovskite films demonstrate a remarkable photon-to-current conversion efficiency improvement of 1.83% for a 330.15 cm2 area SSC device. Additionally, a CHL-modified Yb3+:CsPbCl3 film was used to create 988 nm NIR LEDs with an external quantum efficiency of 3.2%. This work provides a new, eco-friendly approach for producing high-quality, large-area Yb3+-doped perovskite film for deployment in photoelectric and night vision applications.