2D materials possess superior optoelectronic properties, such as ultrahigh mobility and broadband photoresponse, making them one of the most vital platforms for diversified photodetectors. However, atomic thickness 2D materials usually suffer from intrinsic low absorption. To promote the photo detector performance, a feasible method is to integrate the 2D materials with lowcost, flexible, and tunable organics that form a charge transfer (CT) heterojunction. As results, indepth multifunctional CT 2Dinorganic/organic detector exhibits extended functions such as lowpower consumption, in memory detection, and opticalbio synapse to meet the demand of contem porary photonic cell. Particularly, the progresses in waferscale monocrystal of both 2D and organic materials render vast potential applications with operation frequencies ranging from ultraviolet to terahertz. Here, the recent advances of 2Dinorganic/organic CT photodetectors are comprehensively reviewed by several classifications. Future developments and applications in optical biology, synapsis, and machine vision are also highlighted.