transparent, and wearable electronics and optoelectronics due to their reduced dimensions that offer flexibility and transparency with proper band gap, high carrier mobility, and highly efficient light absorption. [1][2][3] In addition, their ideally dangling-bond-free surface and atomic thickness are promising for ideal heterogeneous contact and reduced short channel effect, [4] thus making them suitable for future nano-scaled electronic and optoelectronic devices. An ideal field-effect transistor based on an molybdenum disulfide (MoS 2 ) channel is theoretically predicted to reach large on/off ratio (>10 9 ), room temperature mobility of 410 cm 2 (Vs) −1 , and near-ideal subthreshold swing of 60 meV per decade. [5,6] However, most of experimental results significantly differ from the aforementioned theoretical predictions. One of dominant factors degrading the overall performance of 2D materials based devices arises from unwanted chemical interactions between deposited metal electrodes and 2D TMDC channel. These chemical interactions originate from incomplete/imperfect covalent/surface bonds of TMDCs and unwanted damages from the direct deposition of metal layers and precursors, which are used during the device fabrication processes. These lead to the creation of unfavorable interface states and pinning of fermi energy levels, which Contact engineering for monolayered transition metal dichalcogenides (TMDCs) is considered to be of fundamental challenge for realizing highperformance TMDCs-based (opto) electronic devices. Here, an innovative concept is established for a device configuration with metallic copper monosulfide (CuS) electrodes that induces sulfur vacancy healing in the monolayer molybdenum disulfide (MoS 2 ) channel. Excess sulfur adatoms from the metallic CuS electrodes are donated to heal sulfur vacancy defects in MoS 2 that surprisingly improve the overall performance of its devices. The electrode-induced self-healing mechanism is demonstrated and analyzed systematically using various spectroscopic analyses, density functional theory (DFT) calculations, and electrical measurements. Without any passivation layers, the self-healed MoS 2 (photo)transistor with the CuS contact electrodes show outstanding room temperature field effect mobility of 97.6 cm 2 (Vs) −1 , On/Off ratio > 10 8 , low subthreshold swing of 120 mV per decade, high photoresponsivity of 1 × 10 4 A W −1 , and detectivity of 10 13 jones, which are the best among back-gated transistors that employ 1L MoS 2 . Using ultrathin and flexible 2D CuS and MoS 2 , mechanically flexible photosensor is also demonstrated, which shows excellent durability under mechanical strain. These findings demonstrate a promising strategy in TMDCs or other 2D material for the development of high performance and functional devices including self-healable sulfide electrodes.