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Facing the increasingly serious problem of environmental pollution and energy waste, the thermoelectric generator has been attracting more and more attention owing to its advantages including low cost, no pollution, and good stability. The family of thermoelectric material is constantly extended with enhanced performance. Note that nanostructuring can enhance thermoelectric performance. However, the most recent excellent material with effective thermoelectric transformation reported from bulk materials has definite benefits to the practical application compared to nanomaterials. In this work, a nanostructure integrated macroscale thermoelectric chip, that is an alloyed band gap gradient macroscale chip (1.0 cm × 2.0 cm) composed of CdSSe nanowires, has been proven as an excellent thermoelectric generator for the first time. A high Seebeck coefficient of -152.4 μV/K and the average output voltage of 10.8 mV are obtained after optimizing the electrode patterns and distance between electrodes. More interestingly, upon illumination by white light from a xenon lamp, a photo-thermoelectric output voltage is greatly elevated to 45 mV due to the high concentration of photogenerated carriers. The CdSSe thermoelectric chip also shows good repeatability and high stability with a relative error of <6%. No study on the thermoelectric performance of such an alloyed band gap gradient macroscale chip is mentioned before. The results illustrate a bright avenue to realize a type of light-modulated macroscale thermoelectric chips by nanostructure, allowing such kinds of CdSSe chips to be used to generate electric energy in the near future.