High-entropy sulfides/selenides are expected to be promising anode materials for lithium-ion batteries due to their unique advantages, such as improved electrical conductivity, component adjustability and structural stability. However, the complexity of their preparation makes the morphology/structure regulation of the high-entropy sulfides/selenides more challenging, thus hindering their application in energy storage. In this paper, high-entropy sulfides/selenides with a special yolk–shell structure is designed through a high-entropy precursor vulcanization/selenization strategy. The high-entropy precursors with yolk–shell structure are first prepared by a simple low-temperature solvothermal method, which are transformed to yolk–shell structured high-entropy sulfide ((CrMnFeCoNi)S₂) and selenide ((CrMnFeCoNi)Se₂) by an upstream gas method. Not only do the high-entropy sulfide has a weak short-range order, increasing the ion diffusion channel, but the yolk–shell structure also provides many benefits for lithium-ion batteries, such as enhancing the stability, increasing the ion diffusion rate, and easing the volume expansion. The (CrMnFeCoNi)S₂ electrode exhibits impressive high specific capacity and long cycle life (1375.8 mAh·g⁻¹ after 1250 cycles at 1 A·g⁻¹), and excellent rate capability (1310.6 mAh·g⁻¹ at 2 A·g⁻¹). This research opens a new window of opportunity for developing the next generation of high-entropy compound electrodes for lithium-ion batteries.