Aqueous　aluminum　ion　batteries　(AAIBs)　hold　significant　potential　for　grid-scale　energy　storage　owing　to　their　intrinsic　safety,　high　theoretical　capacity,　and　abundance　of　aluminum.　However,　the　strong　electrostatic　interactions　and　delayed　charge　compensation　between　high-charge-density　aluminum　ions　and　the　fixed　lattice　in　conventional　cathodes　impede　the　development　of　high-performance　AAIBs.　To　address　this　issue,　this　work　introduces,　for　the　first　time,　high-entropy　Prussian　blue　analogs　(HEPBAs)　as　cathodes　in　AAIBs　with　unique　lattice　tolerance　and　efficient　multipath　electron　transfer.　Benefiting　from　the　intrinsic　long-range　disorder　and　robust　lattice　strain　field,　HEPBAs　enable　the　manifestation　of　the　lattice　respiration　effect　and　minimize　lattice　volume　changes,　thereby　achieving　one　of　the　best　long-term　stabilities　(91.2%　capacity　retention　after　10 000　cycles　at　5.0　A　g−1)　in　AAIBs.　Additionally,　the　interaction　between　the　diverse　metal　atoms　generates　a　broadened　d-band　and　reduced　degeneracy　compared　with　conventional　Prussian　blue　and　its　analogs　(PBAs),　which　enhances　the　electron　transfer　efficiency　with　one　of　the　best　rate　performance　(79.2　mAh　g−1　at　5.0　A　g−1)　in　AAIBs.　Furthermore,　exceptional　element　selectivity　in　HEPBAs　with　unique　cocktail　effect　can　facile　tune　electrochemical　behavior.　Overall,　the　newly　developed　HEPBAs　with　a　high-entropy　effect　exhibit　promising　solutions　for　advancing　AAIBs　and　multivalent-ion　batteries.　©　2024　The　Author(s).　Advanced　Materials　published　by　Wiley-VCH　GmbH.