Single-atomic/cluster　metal-based　electrocatalysts　(M-N-C)　is　one　of　the　most　promising　non-noble　metal　catalysts　for　the　oxygen　reduction　reaction　(ORR),　but　their　practical　application　is　severely　hindered　by　insufficient　activity　and　durability.　Herein,　charge　regulation　through　rare　earth　metal　oxides　(REMOs)　for　single-atomic/cluster　metal　based　electrocatalysts　is　proposed　for　boosting　ORR,　in　which　the　Co-based　catalyst　is　taken　as　a　representative　considering　its　typicality　and　universality,　and　CeO2　is　selected　as　representative　after　systematic　computational　screening　from　more　than　10　types　of　REMOs.　As　a　result,　a　novel　REMO-tailored　M-N-C　electrocatalyst　(REMO-Co-N-C)　has　been　successfully　achieved,　which　demonstrates　a　remarkably　increased　activity　and　superior　durability,　namely　a　half-wave　potential　(E₁/₂)　of　0.90　V　and　only　a　loss　of　8　mV　(E₁/₂)　after　10,000　cycles.　Moreover,　in-situ　experiments　and　matched　theoretical　simulations　come　together　organically　to　clearly　and　directly　reveal　the　origin　and　catalytic　behavior　of　the　proposed　electrocatalysts.　Namely　the　charge　regulation　through　REMO　for　M-N-C　can　effectively　modify　the　electronic　structure　of　the　M　sites,　accelerate　the　reaction　rate,　and　enhance　OH*　desorption.　This　work　offers　a　new　insight　for　promoting　M-N-C　catalysts　through　REMO　tailoring,　that　beyond　the　conventional　use　of　d-block　and　p-block　elements.　©　2025　Elsevier　B.V.