Noncovalent interactions play a critical, but not yet understood, role in enhancing the thermoelectric properties of carbon nanotube composites. We herein report the dispersion of synthetic MoS2 flakes and their self-assembly with single-walled carbon nanotubes via in-plane and multipoint S- interactions. The hybridization of MoS2 and carbon nanotubes leads to improved electrical and thermoelectric transport, and resulted in a tenfold enhancement of the thermoelectric figure-of-merit of nanotube-based films. The present technique could contribute to advancing the flexible energy materials that harvest abundant waste heat.