concentration that maximizes the dimensionless thermoelectric (TE) figure of merit ZT (and thus the energy conversion efficiency) of a TE material depends upon the temperature, as illustrated in Figure 1a,b (which derives from expressions detailed in Section S1 of the Supporting Information). ZT is defined as S 2 σT/κ, where S is the Seebeck coefficient, σ is the electrical conductivity, T is the absolute temperature, and κ is the thermal conductivity. The temperature dependence of the optimal carrier concentration poses a challenge since TE devices are typically operated over a wide range of temperatures and, with a fixed carrier concentration, the performance degrades at temperatures for which the carrier concentration is not optimal. This problem is magnified by the fact that the figure of merit is also strongly temperature-dependent and is typically optimized by adjusting the carrier concentration near its peak value. Conventional doping strategies based on adding impurity atoms do not offer a means of controlling the temperature dependence of the carrier concentration because Precise control of carrier concentration in both bulk and thin-film materials is crucial for many solid-state devices, including photovoltaic cells, superconductors, and high mobility transistors. For applications that span a wide temperature range (thermoelectric power generation being a prime example) the optimal carrier concentration varies as a function of temperature. This work presents a modified modulation doping method to engineer the temperature dependence of the carrier concentration by incorporating a nanosize secondary phase that controls the temperature-dependent doping in the bulk matrix. This study demonstrates this technique by de-doping the heavily defect-doped degenerate semiconductor GeTe, thereby enhancing its average power factor by 100% at low temperatures, with no deterioration at high temperatures. This can be a general method to improve the average thermoelectric performance of many other materials.