Porous nanograined thermoelectric materials exhibit low thermal conductivity due to scattering of phonons by pores, which are favorable for thermoelectric applications. However, the benefit is not large enough to overcome the deficiency in the electrical performance. Herein, an approach is presented to reduce the thermal conductivity and synchronously enhance the electrical conductivity through constructing a nanoporous thermoelectric composite. Carbon nanotubes (CNTs) are truncated and homogeneously dispersed within the Bi2Te3 matrix by a cryogenic grinding (CG) technique for the first time, which efficiently suppress the Bi2Te3 grain growth and create nanopores with the size ranging from dozens to hundreds of nanometers. The lattice thermal conductivity is substantially decreased by broad wavelength phonon scattering resulting from nanopores, increased grain boundaries, and newly formed interfaces. Meanwhile, the electrical conductivity is improved due to the enhanced carrier mobility, which may originate from the bridging effect between the Bi2Te3 grains and CNTs. The maximum ZT is improved by almost a factor of 2 due to the simultaneous optimization of electrical and thermal performances. Our study demonstrates the superiority of constructing a bulk thermoelectric composite with nanopores by the uniform dispersion of CNTs through a CG technique for enhanced thermoelectric properties, which provides a wider approach to thermoelectric nanostructure engineering.