Harvesting solar energy to enhance thermoelectric generator efficiency is a highly effective strategy. However, it is a grand challenge but essential to increase solarthermal conversion efficiency. A spectrally selective absorber, which is capable of boosting solar absorptance (α) while suppressing thermal emittance (ε), shows great potential to elevate the solar-thermal conversion efficiency. Herein, we fabricate a multilayer spectrally selective absorber with the assistance of high-entropy nitrides, which shows outstanding spectral selectivity (α/ε = 95.2/10.9%). Benefitting from the high-entropy nitrides, it is experimentally demonstrated that the as-deposited absorber exhibits superior thermal stability, which is crucial to ensure service life. Under 1000 W•m −2 simulated solar illumination, it achieves a very high surface temperature of 109.6 °C, making it suitable to enhance the efficiency of solar thermoelectric generators. Impressively, the integration of the proposed absorber with a commercial thermoelectric generator efficiently reinforces thermoelectric performance, offering a high output power of 1.99 mW. More importantly, by taking advantage of a thermal concentration strategy, it enables a further increase of the output power by 2.98 mW. This work provides a promising solar-thermal material to boost high thermoelectric performance and extends the application category of highentropy nitrides.