Metal-organic　frameworks　(MOFs)　have　undergone　a　rapid　research　expansion　as　unpyrolyzed　oxygen　electrocatalysts　due　to　their　flexible　and　variable　compositions　and　structures.　However,　the　most　studied　MOFs　possess　microporous　nature,　which　limits　the　mass-transfer　properties　and　reduce　the　space　to　store　insoluble　discharge　product　of　aprotic　metal-air　batteries.　We　herein　report　a　partial　ligand　removal　approach　to　create　mesopore　defects　and　unsaturated　coordination　in　primarily　microporous　Cu-BTC　(BTC　=　1,3,5-bezenetricarboxylic　acid).　The　mesopores　were　engineered　by　introducing　isophthalic　acid　as　a　partial　ligand,　which　has　one　carboxylic　group　missing　compared　to　BTC,　to　construct　mesoporous　Cu-BTC　(MCu-BTC).　MCu-BTC　was　further　loaded　by　Co　species　(Co/MCu-BTC)　to　boost　the　bifunctional　catalytic　performance　toward　oxygen　reduction　and　oxygen　evolution　reactions.　The　electrochemical　characterizations　indicate　that　the　mesopores　of　MCu-BTC　enhanced　the　discharging　capacity　(ca.　7000　mAh.g(-1))　of　Co-10/MCu-BTC　in　an　aprotic　Li-air　battery　owing　to　the　mesopores,　which　allowed　electrolyte　infiltration　for　both　mass　and　charge　transfer　and　provided　more　space　to　store　the　discharge　product.　Further　modeling　simulations　shed　light　on　the　contribution　of　the　unsaturated　coordination　by　significantly　promoting　the　electronic　conductivity　and　generating　adequate　interactions　with　reactants,　leading　to　enhanced　mass-　and　charge-transfer　properties.