environmentalmonitoring, infrared imaging, and optical communication. [1,2] Semiconductor nanomaterials and hybrid films (HFs) have attracted much attention for their potential applications in novel photodetectors. [3] In the family of graphene-like 2D materials used in novel optoelectronics, layered transition metal dichalcogenides (TMDs) have a broad application prospect [4][5][6] due to their unique physical features and optoelectronic properties. [7] As a representative material of TMDs, MoS 2 possesses several advantages, including a direct bandgap of ≈1.8 eV, high carrier mobility, and favorable chemical stability, [8] which are especially suitable for sensing light. However, the atomically thin nature of 2D MoS 2 crystals results in an extremely inefficient light-trapping ability, [9] which is a fatal flaw for photodetector devices. The practical application of MoS 2 -based photodetectors is also hindered by severely limited photoresponse and detecting capability, slow response rate, [10] etc. As a result, many efforts have been made to optimize the performance of atomic-layer MoS 2 -based optoelectronics. [10][11][12][13][14][15][16][17][18] Many studies have shown that the use of hybrid photodetectors (HPs) can mitigate the disadvantages of atomically thin MoS 2 crystals. Under the synergistic effect of multimaterials, hybrid MoS 2 -based devices show improved response rates and responsivities. [10][11][12][13][14][15][16][17][18] For example, the photoresponse rate of a MoS 2 -based device increased by almost three orders of magnitude by constructing the heterojunctions with GaSe flakes, [10] and a greatly increased responsivity (10 6 A W −1 ) was achieved in a TiO 2 -encapsulated MoS 2 transistor-modified by HgTe quantum dots. [18] Therefore, a heterojunction structure improves the performance of MoS 2 -based photodetectors, and the successful integration of dissimilar materials may pave the way toward successful high-performance hybrid optoelectronic devices.Currently, lead halide perovskite materials have been widely used in optoelectronic applications, especially solar cells and lightemitting diodes (LEDs), owing to their attractive optoelectronic characteristics, such as high optical absorbance, long diffusion length of charge carriers, and high carrier mobility. [19][20][21] Perovskite materials with different dimensions have been integrated into optoelectronic devices to improve the performance. [22] The past several years have seen the rapid development of fully inorganic trihalide perovskite nanocrystals (PNCs) in the field of hybrid optoelectronic devices due to their outstanding photophysical properties and environmental stability. In this study, novel and easily implementable strategies are proposed to regulate the photoresponse performance of monolayer MoS 2 /PNC hybrid photodetectors (HPs) without the photogating effect. The optoelectronic properties of these HPs are tuned by regulating the characteristic factors of colloidal PNCs (solution concentration and surface ligand content), ...