Rare‐earth‐based high‐entropy alloys (HEAs) with large magnetocaloric effect (MCE) have been recently recognized as good candidates for magnetic refrigeration. Herein, the complex magnetic transition, MCE, refrigerant capacity (RC), and magnetic‐phase diagram of single‐phase TbDyHoEr HEA are studied. It is showed in the results that due to complex magnetic transition and an ideal table‐like MCE, the RC of TbDyHoEr is significantly improved from 883.19 to 1049.22 J kg−1 by melt‐spun treatment. In terms of RC value and hysteresis performance, the melt‐spun treatment significantly improves the application potential of TbDyHoEr HEA as a high‐efficient magnetic refrigeration material, and the ideal table‐like MCE in a large temperature range enables this material to meet the requirements of both cryogenic refrigeration and mesothermal refrigeration for an Ericsson cycle.

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