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Bi2Te3–CNT–PEDOT nanocomposites have been synthesized by mixing PEDOT:PSS with hydrothermally synthesized Bi2Te3–CNT nanocomposites. Introducing conducting interfaces by adding PEDOT in Bi2Te3–CNT boosts the charge carrier mobility, resulting in improved electrical conductivity and simultaneously lowering the lattice thermal conductivity by enhancing phonon scattering and thus resulting in two-fold enhancement of the figure of merit. The detailed mechanism behind the enhancement of charge carrier mobility is discussed by considering the role of conducting interfaces and strong coupling of CNTs and PEDOT conducting chains. The formation of a large number of interfaces in Bi2Te3–CNT–PEDOT nanocomposites acts as strong scattering centers and thermal barriers for long-wavelength phonons, which reduces the lattice thermal conductivity. The formation of interfaces between Bi2Te3 nanostructures and CNT–PEDOT conducting channels has been studied by Kelvin probe force microscopy which clearly showed a smaller interface potential barrier for the Bi2Te3–CNT–PEDOT nanocomposite.