For example, ultrathin flexible electrode arrays could be installed on epidermis [16] or organ surfaces [17] for real-time monitoring of human health that cannot be realized by traditional rigid electronic devices. Thus, new functional materials of flexible electronics that not only meet the demand of high performance but also have good stability and durability under reiterative bending, folding, or stretching are urgently pursued.2D transition metal dichalcogenides (2D TMDs) are a rising star in the family of 2D layered materials since their outstanding electrical and optical properties, such like tunable bandgaps, [18] high absorbance, [19] quick carrier generation, and migration. [20] More importantly, 2D TMDs materials are featured by strong covalent intralayer bonds and weak van der Waals (vdW) interlayer bonding, which make them a promising candidate to build atomicscale or nanoscale Lego devices as well as flexible electronics applications. [21][22][23] Studies have shown that covalent bond can tolerate enormously higher strains (up to 40%) than ionic bonded bulk forms (≈18%), which can enable 2D TMDs sustain the deformation over 10% before rupture, [24] while the fracture value of typical bulk semiconductors is usually less than 1%. [25] Besides, according to the dependence of the stiffness (k) on cross-section (A) and length (L) expressed as k = E × A/L, 2D TMDs are expected to have excellent flexibility with a very low k due to their ultrathin thicknesses. [26] Layered molybdenum disulfide (MoS 2 ), as a semiconductor material with an indirect bandgap of 1.2-1.8 eV (direct bandgap in monolayer materials), has been employed in lots of photoelectronic devices. Up to now, substantial developments and progresses concerned have been witnessed, especially on flexible photodetectors owing to its terrific mechanical flexibility with 11% stretch. [27] Its reducible atomic thickness greatly facilitates the design and construct for bending, crimping, and folding, whereas it comes at the expense of excellent optoelectronic properties. [28] The carrier mobilities of MoS 2 on flexible substrates range from 4.7 to 45 cm 2 V −1 s −1 , [29] while that on Si substrate is up to 480 cm 2 V −1 s −1 . [30] The high variation should be caused by introducing impurities and creating sources of extrinsic scattering in physical contacts, which reduces the mean-free path of the carriers. [31] The latest researches show that, the synergetic integration of two layered materials is a promising strategy to overcome the shortages of individual Flexible electronics is one of the hotspots of interdisciplinary research and can promote disruptive technology for post-Moore applications in the field of biomedical, electronic skin, wearable devices, etc. 2D materials have triggered great interest in flexible electronic devices since they have tunable bandgaps, excellent mechanical flexibility, good chemical stability, and outstanding optical properties. Their reducible atomic thickness greatly facilitates the design and construct for bending,...