The　development　of　high-performance　cathode　materials　is　of　great　importance　for　aqueous　alkaline　Zn　batteries　(AZBs)　but　also　remains　a　great　challenge.　Herein,　we　demonstrate　the　rational　design　and　synthesis　of　NiCo2S4　nanoparticles　and　hollow　carbon　hybrid　spheres　compactly　concatenated　by　carbon　fibers　(denoted　as　NiCo2S4/HCS@CFs)　through　an　innovative　combination　of　metal-organic　framework　(MOF)-derived　strategy　and　electrospinning　technique.　The　as-synthesized　NiCo2S4/HCS@CF　film　is　flexible,　lightweight,　and　free　of　any　polymer　binders,　which　offers　multilevel　advantages　including　high　electrical　conductivity,　abundant　electroactive　sites,　fast　ion　diffusion,　facile　electrolyte　permeability　and　robust　structural　stability.　When　evaluated　as　self-standing　cathode　electrodes,　as　expected,　the　resulting　NiCo2S4/HCS@CFs//Zn　batteries　exhibit　an　extremely　high　capacity　of　343.1　mA　h　g(-1)　at　a　current　density　of　3.8　A　g(-1)　(based　on　the　NiCo2S4　active　material),　as　well　as　superior　rate　performance　and　decent　cycling　performance.　Moreover,　the　corresponding　quasi-solid-state　batteries　are　also　fabricated　to　confirm　the　potential　for　practical　applications.　Remarkably,　the　energy　densities　of　NiCo2S4/HCS@CFs//Zn　batteries　are　563.2　W　h　kg(-1)　and　49.1　mW　h　cm(-3)　(liquid)　and　504.1　W　h　kg(-1)　and　43.9　mW　h　cm(-3)　(quasi-solid-state).　What＇s　more,　density　functional　theory　(DFT)　calculations　reveal　that　NiCo2S4/HCS@CFs　have　strong　adsorption　ability　for　OH-　ions.　This　work　not　only　highlights　the　importance　of　developing　advanced　flexible　and　lightweight　cathode　electrodes　for　aqueous　AZBs,　but　also　provides　some　insights　into　electrode　designs　for　other　energy　storage　devices.