We report a strategy to realize and facilitate the photocarrier transport from mercury selenium colloidal quantum dots (HgSe CQDs) into silicon with the assistance of twisted graphene. A nanocomposite material consisting of HgSe CQDs and twisted graphene has been synthesized. By bringing the nanocomposites into contact with silicon, a HgSe CQD-twisted graphene nanocomposite/silicon junction was fabricated and demonstrated photoresponses in the long-wave infrared range. In the nanocomposites, the surface of twisted graphene was decorated with HgSe CQDs. Benefiting from the twisted structure in the nanocomposites, the active sensing area and light-matter interaction length are greatly increased. Driven by the interfacial built-in potential, photocarriers directly transfer from HgSe CQDs into the twist graphene, which serves as a fast carrier transport pathway to silicon, leading to high photocarrier collection efficiency. Compared with vertically stacked HgSe CQD film/flat graphene, the application of HgSe CQD-twisted graphene nanocomposites avoids photocarriers transporting via the hopping mechanism and over 2700% enhancement ratio of spectral responsivity was achieved, reaching 31.5 mA/W@9 μm. The interfacial energy band diagram was deduced for a better understanding of the photocarrier transfer process occurring at the interface between HgSe colloidal quantum dots, twist graphene, and silicon.