Searching　for　high-performance　Ni-based　cathodes　plays　an　important　role　in　developing　better　aqueous　nickel-zinc　(Ni-Zn)　batteries.　For　this　purpose,　herein,　we　demonstrate　the　design　and　synthesis　of　ultrathin　α-Ni(OH)2　nanosheets　branched　onto　metal-organic　frameworks　(MOFs)-derived　3D　cross-linked　N-doped　carbon　nanotubes　encapsulated　with　tiny　Co　nanoparticles　(denoted　as　Co@NCNTs/α-Ni(OH)2),　which　are　directly　supported　on　a　flexible　carbon　cloth　(CC).　An　aqueous　Ni-Zn　battery　employing　the　hierarchical　CC/Co@NCNTs/α-Ni(OH)2　as　the　binder-free　cathode　and　a　commercial　Zn　plate　as　the　anode　is　fabricated,　which　displays　an　ultrahigh　capacity　(316　mAh　g-1)　and　energy　density　(540.4　Wh　kg-1)　at　1　A　g-1　as　well　as　excellent　rate　capability　(238　mAh　g-1　at　10　A　g-1)　and　superior　cycling　performance　(about　84%　capacity　retention　after　2000　cycles　at　10　A　g-1).　The　impressive　electrochemical　performance　might　benefit　from　the　rich　active　sites,　rapid　electron　transfer,　cushy　electrolyte　access,　rapid　ion　transport,　and　robust　structural　stability.　In　addition,　the　quasi-solid-state　CC/Co@NCNTs/α-Ni(OH)2//Zn　batteries　are　also　successfully　assembled　with　polymer　electrolyte,　indicating　the　great　potential　for　portable　and　wearable　electronics.　This　work　might　provide　important　guidance　for　constructing　carbon-based　hybrid　materials　directly　supported　on　conductive　substrates　as　high-performance　electrodes　for　energy-related　devices.　©　2021　American　Chemical　Society.