Previous　theoretical　calculations　have　predicted　that　the　incorporation　of　tellurium　(Te)　into　carbon　materials　can　significantly　enhance　their　catalytic　activity.　Nevertheless,　the　experimental　realization　of　efficient　Te-doped　carbon　materials　remains　challenging.　Here,　we　employed　theoretical　calculations　to　deduce　the　possible　structure　of　Te-doped　carbon　materials.　Our　findings　unveil　that　the　formation　of　Te-O　pairs　in　carbon　materials　with　a　relatively　low　oxygen　coordination　microenvironment　can　impart　strong　electron-donating　capabilities,　thereby　boosting　the　electrocatalytic　activity　of　oxygen　reduction　reaction　(ORR).　To　verify　our　theoretical　predictions,　we　synthesized　Te-O　pair-doped　carbon　materials　using　a　tandem　hydrothermal　dehydration-pyrolysis　strategy.　This　approach　enabled　efficient　infiltration　of　Te　into　carbon　materials.　Our　unconventional　Te-O　pair-doped　carbon　materials　exhibit　expanded　interlayer　distances　and　graphene-like　nanosheet　architectures,　which　provide　enlarged　active　areas.　These　structural　features　contribute　to　the　enhanced　ORR　catalytic　performance　of　the　as-prepared　carbon　catalyst.　Our　findings　provide　molecular-level　insights　into　the　design　of　various　carbon-based　with　active　sites.