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To achieve chromium tolerance and high performance, a new series of high-entropy perovskites (HEPs) are investigated as cathode materials for solid oxide fuel cells (SOFCs). Multiple rare-earth, alkaline-earth, and high-order transition metal elements are used for the A-site of this ABO₃ structure. A pure phase is achieved through the designed combination of different elements in seven out of eight candidates. Due to the retaining of alkaline-earth elements Sr and/or Ba, the electrical conductivities of these HEPs are in the order of 100 S/cm at 550–700 °C, a value that can practically eliminate the electronic resistance of the porous cathode. Three out of eight candidates show similar or better performance than the (La_0.6Sr_0.4)(Co_0.2Fe_0.8)O_3−δ (LSCF) benchmark. It is found that A-site elements can cast a substantial influence on the overall performance even with a change as small as 10% of the total cations. It …