Unique hollow hybrid structures composed of well-dispersed catalyst nanoparticles embedded in a carbon matrix offer great advantages for constructing advanced supported catalysts. Herein, we report the designed synthesis of Co₉S₈ and nitrogen doped hollow carbon sphere (Co₉S₈/NHCS) composites by carbonization of metanilic anions within the confinement of two-dimensional galleries of hollow spherical cobalt–aluminum layered double hydroxides. The Co₉S₈/NHCS composites are composed of numerous porous carbon nanoflakes, and monodisperse Co₉S₈ nanoparticles are embedded within the carbon nanoflakes. Electrochemical measurements show that the Co₉S₈/NHCS catalysts prepared at 900 °C exhibit superior oxygen reduction reaction (ORR) activity, resulting in the highest ORR performance to date among all transition metal sulfide-based ORR catalysts in both alkaline and acidic electrolytes. This interlayer confined reaction approach may provide an efficient platform for the synthesis of other functional materials for alternative applications.