2D transitional metal dichalcogenide (2D-TMDC) materials, as inorganic graphene analogs (IGAs), have been intensively investigated for their novel chemical and physical properties when the thickness is reduced to a few atomic layers, such as MoS 2 , WS 2 , among others. [1] Tantalum disulfide, TaS 2 , one of the TMDC materials, has attracted growing attention recently. In the bulk state, TaS 2 occupies 2H or 1T structure, which is composed of covalently bonded STaS layers. 1T-TaS 2 with Ta in octahedral coordination with S atoms exhibits semiconducting behavior, and it has a commensurate charge density wave (CCDW) phase under 180 K. Adjusted by pressure, the superconductivity of 1T-TaS 2 develops in the CCDW state and survives to very high pressure. [2][3][4] 2H-TaS 2 with Ta in trigonal prismatic coordination with S atoms exhibits metallic behaviors with CDW phase transition (T CDW = 75 K) and superconductivity (T c = 0.8 K). [5][6][7][8] The electrical conductivity of single-crystal 2H-TaS 2 can reach 6.8 × 10 4 S m −1 at room temperature. [9] When the thickness is reduced to a few layers, interesting phenomena have been found, such as gate-tunable phase transition [10] and enhanced superconductivity, [11] which are promising properties for applications like electrical oscillators, [12] fast memories, [13] hydrogen evolution catalyst. [14] Until now, 2D TaS 2 has been mainly synthesized by the mechanical exfoliation method, [15] which is time consuming and of poor reproductivity and low yield. It has been noticed that the exfoliation of TaS 2 seems rather difficult and the atomically thin layers are unstable in ambient environments due to easy oxidation. [16] Complex encapsulation techniques are therefore required to help preserve the samples in air. [16] The chemical vapor deposition method [17] proves to be swift and effective in fabrication of high-quality 2D materials, but large-area synthesis of full-coverage atomically thin material is still in progress. For device applications, solution-based chemical synthesis is particularly important, as the product can be easily integrated into electronic devices.There is a new solution-based strategy to synthesize 2D materials in the form of inorganic/organic superlattice, in which the inorganic layers may get close to the low-dimensional state due to the spatial separation by the organic molecules. In our previous papers, we synthesized a hybrid superlattice with alternating 2D [TiS 2 ] monolayers and organic cations through an electrochemical reaction process. [18] The isolation of the [TiS 2 ] TaS 2 nanolayers with reduced dimensionality show interesting physics, such as a gate-tunable phase transition and enhanced superconductivity, among others. Here, a solution-based strategy to fabricate a large-area foil of hybrid TaS 2 /organic superlattice, where [TaS 2 ] monolayers and organic molecules alternatively stack in atomic scale, is proposed. The [TaS 2 ] layers are spatially isolated with remarkably weakened interlayer bonding, resulting in lattice vibration ...