Synthesis　of　nanostructured　composites　containing　multiple　components　with　distinctive　structure　and　composition　is　important　for　high-performance　energy　storage　but　challenging.　Starting　form　metal-organic　frameworks　(MOFs),　we　herein　successfully　synthesize　a　series　of　advanced　nanocomposites　consisting　of　composition-tailored　nickel　cobalt　sulfoselenide　(NiCo2(SxSe1−x)5)　nanoparticles　confined　in　graphitic　carbon　hollow　spheres　(GC　HSs).　For　pseudocapacitors,　the　NiCo2(S0.78Se0.22)5/GC　HSs　exhibit　the　highest　specific　capacity　(560.7　C　g−1　at　1　A　g−1)　with　good　rate　capability　and　cycling　performance.　An　asymmetric　supercapacitor　(ASC)　based　on　the　NiCo2(S0.78Se0.22)5/GC　HSs　cathode　and　Bi2O2.33/rGO　nanocomposite　anode　displays　an　energy　density　of　47.2　Wh　kg–1　at　a　high　power　density　of　801　W　kg–1.　Besides,　the　NiCo2(S0.78Se0.22)5/GC　HSs　are　also　promising　anode　materials　for　lithium-ion　batteries,　which　deliver　a　high　reversible　capacity　of　865.2　mA　h　g−1　at　200　mA　g−1　after　100　cycles.　The　excellent　performance　could　be　attributed　to　the　high　electrical　conductivity,　facile　electron　and　ion　transport,　good　structural　robustness　and　components’　synergistic　effect.　We　believe　this　synthetic　strategy　could　be　extended　to　prepare　other　anions　doped　bimetallic　compounds　and　carbon　composites　for　next-generation　energy　storage.　©　2018　Elsevier　B.V.