Harnessing individual electronic and thermal transport properties selectively has long been a fundamental goal of achieving high thermoelectric (TE) performance in many materials. TE energy conversion efficiency of materials is directly proportional to the material-dependent parameter as known as a dimensionless figure of merit, zT. In principle, twofold intercorrelated relations of physical parameters i) between electrical conductivity (σ) and Seebeck coefficient (S) and ii) between σ and total thermal conductivity (κ total ) in TE semiconductors are strongly correlated each other and the trade-offs have been major obstacles for improving zT, which is determined by zT = S 2 σ T/κ total where T is temperature and κ total consists of the sum of electronic (κ elec ) and lattice (κ latt ) contributions to thermal conductivity.Many efforts have been demonstrated to overcome these long historic cliché issues on thermoelectrics. Concerning about electronic transports, several distinct strategies have been proposed for exclusively enhancing power factor (PF: S 2 σ) by utilizing resonance state in Tl-doped p-type PbTe, [1,2] the convergence of electronic bands, [3] and the doping modulation in nanocomposites. [4] However, these approaches are not widely applicable to all TE materials since the enhancement of PF through such strategies utterly depends on the unique electronic band structure of the individual material. Apart from the optimization of PF, remarkable enhancements of the zT have been achieved mostly due to the reduction of the κ latt via increased phonon scattering utilizing structural defects in nanostructured materials, such as grain boundaries, interfaces, dislocations, and precipitates. [4][5][6][7] Further, efforts to find a new material with intrinsically low thermal conductivity have been devoted. [8][9][10] In fact, little room remains for further reducing κ latt in nanostructured single-phase materials because κ latt cannot be reduced below the amorphous limit, which has been already achieved in the state-of-the-art nanostructured TE materials. Moreover, it has been widely recognized that κ elec cannot be decoupled from σ. However, there is a possibility to reduce the κ elec value by decreasing Lorenz number (L) since L is a band structure-dependent parameter of material but relatively Taming electronic and thermal transport properties is the ultimate goal in the quest to achieve unprecedentedly high performance in thermoelectric (TE) materials. Most state-of-the-art TE materials are inherently narrow bandgap semiconductors, which have an inevitable contribution from minority carriers, concurrently decreasing Seebeck coefficient and increasing thermal conductivity. Nevertheless, the restraint control of minority carrier transport is seldom considered as a key element to enhance the TE figure of merit (zT). Herein, it is verified that the localized dislocation arrays at grain boundaries enable the suppression of minority carrier contribution to electronic transport properties, resulting in an increase ...