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Few-layer MoS2films stay at the forefront of current research of two-dimensional materials. At present, continuous MoS2films are prepared by chemical vapor deposition (CVD) techniques. Herein, we present a cost-effective fabrication of the large-area spatially uniform films of few-layer MoS2flakes using a modified Langmuir–Schaefer technique. The compression of the liquid-phase exfoliated MoS2flakes on the water subphase was used to form a continuous layer, which was subsequently transferred onto a submerged substrate by removing the subphase. After vacuum annealing, the electrical sheet resistance dropped to a level of 10 kΩ/sq, being highly competitive with that of CVD-deposited MoS2nanosheet films. In addition, a consistent fabrication protocol of the large-area conductive MoS2films was established. The morphology and electrical properties predetermine these films to advanced detecting, sensing, and catalytic applications. A large number of experimental techniques were used to characterize the exfoliated few-layer MoS2flakes and to elucidate the formation of the few-layer MoS2Langmuir film.