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Elemental engineering has been employed to adjust molecular framework and electronic configuration of γ-graphyne for rapid lithium storage. Here, we construct a quasi-pyridinic nitrogen/sulfur co-doped γ-graphyne (N/S-GY) via a mechanochemical strategy and reveal its lithium storage behavior by quantitative kinetics analysis and theoretical calculations. The internal pyridinic-N atoms create rhombic channels for Li+ passing through, while sulfur dopants anchored with alkynyl groups induce electron cloud rearrangement to facilitate intralayer Li+ diffuse between C 12 -triangular channels and interlayer transfer through open rhombic channels. As a result, the as-prepared N/S-GY exhibits a high reversible capacity of 1003 mAh g−1 at 50 mA g−1 after 150 cycles, with Li+ diffusion coefficient up to 2.6 × 10−12 cm2 s−1, both of which are larger than that of N-doped γ-graphyne. This work highlights synergistic effect of sulfur and nitrogen co-doping in alkynyl carbon and inspires bottom-up heteroatom modification in framework design. [Display omitted] • Sulfur and nitrogen co-doped γ-graphyne has been prepared through a mechanochemical route. • The N/S-GY anode displays high lithium-ion capacity with 1003 mAh g−1 at 50 mA g−1 after 150 cycles. • The N/S-GY anode exhibits lithium diffusion efficiency with 2.6 × 10−12 cm2 s−1. [ABSTRACT FROM AUTHOR]