Thermoelectric technology, reversibly converting heat into electricity, faces application dilemmas due to high costs and the scarcity of Te. Herein, cost-effective n-type PbSe crystals prepared by physical vapor deposition exhibit potential for power generation and refrigeration. Carrier density and mobility of the PbSe crystals are both increased by lattice plainification via adding trace In and Sb, leading to a significant PF of 40 μW cm –1 K –2 at 303 K. The lattice mismatch and enlarged bandgap prominently lower the lattice thermal conductivity. The distinguished ZT s of 0.6 and 1.6 are realized at 303 and 773 K ( ZT ave = 1.14 across 303–773 K), respectively. Furthermore, a 17-pair thermoelectric cooling module is assembled with Pb 1.003 In 0.0006 Sb 0.0006 Se and realizes a cooling temperature difference of 55 K ( T h = 343 K). Meanwhile, a segmented single-leg device is manufactured with Pb 1.003 In 0.0012 Sb 0.0012 Se and Pb 1.003 In 0.0006 Sb 0.0006 Se, achieving an eminent conversion efficiency of 10% with a Δ T of 470 K.