Selenium–sulfur solid solutions are a class of potential cathode materials for high energy batteries, since they have higher theoretical capacities than selenium and improved conductivity over sulfur. Here, a high‐performance cathode material by confining 70 wt% of SeS 2 in a highly ordered mesoporous carbon (CMK‐3) framework with a polydopamine (PDA) protection sheath for novel Li–Se/S batteries is reported. With a relatively high SeS 2 mass loading of 2.6–3 mg cm −2 , the CMK‐3/SeS 2 @PDA cathode exhibits a high capacity of >1200 mA h g −1 at 0.2 A g −1 , excellent C‐rate capability of 535 mA h g −1 at 5 A g −1 , and prolonged life over 500 cycles. Benefitting from the unique advantages of SeS 2 and the rationally designed host framework, this new cathode material demonstrates a feasible strategy to overcome the bottlenecks of current Li–S systems for high energy density rechargeable batteries.