Directly　growing　nickel/cobalt-based　cathode　materials　on　current　collectors　as　binder-free　electrodes　for　rechargeable　aqueous　nickel/cobalt-Zn-based　(NiCo//Zn)　batteries　have　attracted　tremendous　attentions.　However,　most　of　the　present　binder-free　cathodes　suffer　from　low　areal　capacity　and　energy　density,　which　severely　restrict　their　practical　applications.　Herein,　we　demonstrate　an　efficient　metal-organic　framework　(MOF)-involved　strategy　to　rationally　integration　of　the　active　NiCo2O4,　CoMoO4　and　Co3O4　cathode　materials　into　one　hierarchical　arrayed　structure　that　uniformly　grown　on　nickel　foam　(NF)　substrate　(denoted　as　NF–NCO@CMO@CO)　with　a　high　mass　loading　of　9.6　mg　cm−2.　Such　electrode　design　possesses　favorable　merits　in　the　aspects　of　high　electrical　conductivity,　robust　arrayed　architectures,　abundant　electrochemical　active　sites,　rich　redox　reactions,　facile　ion　diffusion　and　components’　synergetic　effect.　As　a　result,　the　aqueous　NiCo//Zn　battery　based　on　NF–NCO@CMO@CO　binder-free　cathode　exhibits　an　ultrahigh　areal　capacity　of　2.51　mAh　cm−2　at　a　current　density　of　2　mA　cm−2,　as　well　as　good　rate　capability　and　long-term　cycling　stability.　Impressively,　the　aqueous　NF–NCO@CMO@CO//Zn　battery　shows　a　maximum　areal　energy　density　of　4.09　mWh　cm−2　(corresponding　to　424.5　Wh　kg−1),　which　is　superior　to　most　of　the　previously　reported　aqueous　NiCo//Zn　batteries.　Electrode　reaction　kinetics　analysis　reveals　that　both　capacitive　and　diffusion-controlled　behaviors　are　involved　during　the　charge　storage　processes.　Moreover,　a　quasi-solid-state　NF–NCO@CMO@CO//Zn　battery　is　also　assembled　by　replacing　the　liquid　electrolyte　with　gel　electrolyte,　suggesting　the　potential　for　practical　applications.　This　work　might　shed　light　on　the　rational　construction　of　advanced　binder-free　cathodes　for　high-performance　aqueous　NiCo//Zn　batteries.　©　2020　Elsevier　B.V.