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Single-walled carbon nanotube (SWCNT)-based thermoelectric materials have been extensively studied in the field of flexible wearable devices due to their high flexibility and excellent electrical conductivity (σ). However, poor Seebeck coefficient (S) and high thermal conductivity limit their thermoelectric application. In this work, free-standing MoS2/SWCNT composite films with improved thermoelectric performance were fabricated by doping SWCNTs with MoS2nanosheets. The results demonstrated that the energy filtering effect at the MoS2/SWCNT interface increased the Sof composites. In addition, the σ of composites was also improved due to the reason that S–π interaction between MoS2and SWCNTs made good contact between MoS2and SWCNTs and improved carrier transport. Finally, the obtained MoS2/SWCNT showed a maximum power factor of 131.9 ± 4.5 μW m–1K–2at room temperature with a σ of 680 ± 6.7 S cm–1and an Sof 44.0 ± 1.7 μV K–1at a MoS2/SWCNT mass ratio of 15:100. As a demonstration, a thermoelectric device composed of three pairs of p–n junctions was prepared, which exhibited a maximum output power of 0.43 μW at a temperature gradient of 50 K. Therefore, this work offers a simple method of enhancing the thermoelectric properties of SWCNT-based materials.