A molecular layer of an organo europium (Eu) complex was hybridized with the surface of halide perovskite (MAPbI3) nanocrystals to control charge transport between photoexcited perovskites and a metal electrode. A thin hybridized nanocrystalline film was found to cause an efficient photomultiplication reaction based on hole accumulation at photoexcited perovskite nanoparticles and charge tunneling across the Eu complex molecules under application of a low external bias (-0.5 V). A photodetecting device based on the Eu complex and perovskite absorber demonstrated photoinduced current generation at extremely high quantum conversion efficiency of 290 000% for weak monochromatic light (<1 mW cm-2), yielding a power responsivity value up to 1289 A W-1. High sensitivity of photodetection was enabled by using nanosized particles (<5 nm) of perovskite having a high surface area in contact with the Eu complex, while sensitivity was reduced by use of thick and large particle perovskite layers.