Abstract 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 close to that of TaS 2 monolayers. The foil also shows excellent mechanical flexibility together with a large electrical conductivity of 1.2 × 10 3 S cm −1 and an electromagnetic interference of 31 dB, among the highest values for solution‐processed thin films of graphene and inorganic graphene analogs. The solution‐based strategy reported herein can add a new dimension to manipulate the structure and properties of 2D materials and provide new opportunities for flexible nanoelectronic devices.