have received considerable attention for their potential applications in future electronic and optoelectronic devices (e.g., transistors, photodetectors, sensors, and solar cells). [5][6][7][8][9][10] However, for photo detection applications, individual 2D materials do not possess sufficiently high responsivity (R), fast response time (τ), and broadband working bandwidth simultane ously. For example, photodetectors based on gapless pristine graphene display very fast time response and broadband detec tion spectra, but their responsivity is lim ited to a level of mA·W −1 , due to the low light absorption rate and fast electron-hole recombination in graphene. [8,[11][12][13] Photo detectors based on molybdenum disulfide (MoS 2 ) show a high photoresponsivity of ≈880 A·W −1 , but their response time is rel atively long due to the long life time of their photocarriers, and their working wave length is limited to the visible spectrum due to the large bandgap of MoS 2 . [14,15] Considering the high carrier mobility inside graphene, [16,17] an effective method of building highperformance photodetectors is to interface gra phene with lightabsorbing materials, such as quantum dots, [18] perovskites, [19] TMDCs, [20] organic heterostructure, [21,22] sil icon, [23] etc. Among these graphenebased van der Waals (vdW) heterostructures, photodetectors consisting of only atomically thin 2D materials are particularly attractive for their possibility to form a sandwich structure for ultraflexible and highperfor mance electronic and optoelectronic applications. [24] However, these types of graphenebased devices consisting of only one layer of 2D crystals also suffer from the tradeoff between photo responsivity (R) and response time (τ). For example, graphene MoS 2 heterostructurebased photodetectors show enhanced photoresponsivity (≈5 × 10 8 A·W −1 ) at the expense of extremely slow response times (≈1 × 10 3 s). [20] The absence of an internal electric field within the lightabsorption layer can cause low photo carrierseparation efficiency, thus resulting in low quantum efficiency (QE) and relatively long response times (typically in the range of seconds, without gating pulses). [20] Although several strategies (e.g., the use of a ferroelectric sub strate [25] or a top transparent electrode [18] ) artificially introduce an external electric field to facilitate charge separation, these approaches are highcost and require complex fabrication pro cesses. Furthermore, most of these photodetectors display a Integrating 2D crystals into optical fibers can grant them optoelectronic properties and extend their range of applications. However, the ability to produce complicated structures is limited by the challenges of chemical vapor deposition manufacturing. Here, a 2D-material heterostructure created on a fiber end-face is successfully demonstrated by integrating a microscale multilayer graphene-MoS 2 -WS 2 heterostructure film on it, using a simple layer-by-layer transferring method. The all-in-fiber photodetector (FPD) exhibits an ultra...