摘要： Graphene is an attractive material for photodetection and optoelectronic applications because it offers a broad spectral bandwidth and ultrafast response speed. However, because of the broad light absorption characteristic, graphene has a lack of selectivity to the wavelength, which limits the performance of graphene-based photodetectors. Here, we demonstrate a novel hybrid photodetector with monolayer graphene covered with an ultrathin film of surface covalent organic frameworks (COFs) with variable structures as the light-harvesting materials. Photodetectors based on surface COF?G show enhanced responsivity in comparison with unmodified graphene and graphene modified with monomers. The submolecular resolution of scanning tunneling microscopy allows us to get a direct insight into the relationship between the microscopic interfacial structure and the performance of the device. We prove that the enhancement in the device performance is directly related with the orderliness of surface COFs, which influences the interfacial charge transfer by tuning π?π stacking between surface COF and graphene.