transition metal dichalcogenides (TMDs), which present indirect bandgaps in the range of 1.0-2.0 eV and are suitable for electronic devices. [1] Molybdenum disulfide (MoS 2 ) is the one of the most explored TMDs, ideal for new generation electronics, [2] optoelectronics, [3] and topological insulators. [4] Several examples of applications can be found where MoS 2 thin films are used, such as sensors, [5] energy storage, [6] or flexible electronics. [7] Thus, a method to prepare highly concentrated and stable dispersions of excellent quality semiconducting TMDs materials is essential in order to achieve solutionprocessed, inexpensive, large area high performance devices.However, exfoliated MoS 2 flakes exhibit heterogeneous properties, depending on their thickness, lattice structures as well as chemical composition. The synthetic methods are thus critically important, in order to access their intact properties. Considerable progress have been achieved to overcome the weak interlayer interactions to produce mono-or few-layer MoS 2 using micromechanical cleavage, [2,8] chemical intercalation, [9] and ultrasound-promoted shear exfoliation. [10] While micromechanical cleavage is able to obtain pristine MoS 2 flakes with very limited yield, the chemical routes using harsh tert-butylithium-mediated intercalation are able to produce single-layer MoS 2 flakes with large quantity. However, the lithium intercalation converts MoS 2 from pristine semiconducting 2H phase to metallic 1T phase. Beyond that, liquid-phase exfoliation with suitable solvents (e.g., N-methyl-2-pyrrolidone (NMP)) offers macroscopic quantity of 2H-MoS 2 flakes. [11] Nonetheless, it requires long-last agitation (e.g., 23 h) and delivers low exfoliation yields (≈40%) as well as small sheet sizes (less than 1 µm). [12] By now, it remains a great challenge to prepare large sheet size, high-quality 2H-MoS 2 flakes with high yield.Herein, we demonstrated a novel scalable method to prepare high-quality 2H-MoS 2 flakes by cathodic exfoliation in organic electrolyte. Especially, the intercalation of tetra-n-butylammonium cations in bulk MoS 2 benefits to fast exfoliation within 1 h, high yield of 70% and large-sized flakes up to 50 µm. The method is appealing to obtain high quality multiflake films with no throughput limitations for the variety of electronic applications abovementioned. As a first application, we fabricated the large-area biosensor, developed by a restacking the 2H-MoS 2 flakes into thin film on the flexible polyimide 2D molybdenum disulfide (MoS 2 ) gives a new inspiration for the field of nanoelectronics, photovoltaics, and sensorics. However, the most common processing technology, e.g., liquid-phase based scalable exfoliation used for device fabrication, leads to the number of shortcomings that impede their large area production and integration. Major challenges are associated with the small size and low concentration of MoS 2 flakes, as well as insufficient control over their physical properties, e.g., internal heterogeneity of the metal...