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A graphited g -C 3 N 4 assembled with highly-dispersed nickel (HDNi@ g -C 3 N 4) exhibits accelerated reaction kinetics, excellent reversible capacity, and rate performance due to superior metallicity with increased density of states (DOS) at the Fermi energy level, narrowed energy gap between LUMO and HOMO level, and decreased positive Gibbs energy of polysulfide conversion. [Display omitted] • A graphited g -C 3 N 4 assembled with highly-dispersed nickel is designed as a catalyst of Li-S battery. • Exhibiting superior metallicity with increased density of states (DOS) at the Fermi energy level. • Narrowed energy gap contributes much to fast kinetics of negative electrons and positive Li+ ions. • Positive Gibbs energy significantly decreases for the prepared cathode materials. Lithium-sulfur (Li-S) batteries are promising next-generation energy storage devices due to high theoretical energy density and low-cost. Nevertheless, the practical applications are hindered by polysulfide shuttling effect, low electrical conductivity of sulfur, and slower conversion kinetics. Here, the graphited g -C 3 N 4 assembled with highly-dispersed nickel (HDNi@ g -C 3 N 4) is designed as a catalyst to accelerate the reaction kinetics of lithium polysulfide. The oxidized Ni sites of HDNi@ g -C 3 N 4 molecules significantly accommodate the orbital for the electron clouds of polysulfide by forming S n 2–‧‧‧Ni-N active site, thus efficiently improving redox kinetics and mitigating shuttle effects. Based on density functional theory (DFT) calculations, HDNi@ g -C 3 N 4 exhibits a superior metallicity with increased density of states (DOS) at the Fermi energy level. Then, the narrowed energy gap between the lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) level contributes to the enhanced conductivity of catalyst molecular and fast combination between electrons and Li+ ions. Moreover, the positive Gibbs free energy change is significantly decreased for the HDNi@ g -C 3 N 4 cathode. The Li-S battery exhibits a high reversible capacity of 1, 271.6 mAh g−1 at 0.1 C and a high rate capacity of 571.96 mAh g−1 at 2.0 C, a preferable cycling stability with a capacity retention of 53 % even after 500 cycles at a 1.0 C, and an average decay rate of 0.733 % per cycle. [ABSTRACT FROM AUTHOR]