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Developing materials that possess high electrical conductivities (σ) and Seebeck coefficients (S), low thermal conductivities (κ), and excellent mechanical properties is important to realize practical thermoelectric (TE) devices. Here, 3D hierarchical architectures consisting of hybrid molybdenum disulfide (MoS2)/carbon nanotubes (CNTs) films are fabricated with the goal of increasing σ and decreasing κ. In these films, perpendicularly orientated CNTs interpenetrate restacked MoS2 layers to form a 3D architecture, which increases the specific surface area and charge concentration. The MoS2/20 wt% CNTs film shows high σ (235 ± 5 S∙cm−1), high S (68 ± 2 µV∙K−1), and low κ (19 ± 2 mW∙m−1∙K−1). The corresponding figure of merit (ZT) reaches 0.17 at room temperature, which is 65 times higher than that of pure MoS2 film. In addition, the MoS2/20 wt% CNTs film shows a tensile stress of 38.9 MPa, which is an order of magnitude higher than that of a control MoS2 film. Using the MoS2/CNTs film as an active material and human body as a heat source, a flexible, wearable TE wristband is fabricated by weaving seven strips of the 3D porous MoS2/CNTs film. The wristband achieves an output voltage of 2.9 mV and corresponding power output of 0.22 µW at a temperature gradient of about 5 K.