Elevating Lithium and Sodium Storage Performance Through the Synergistic Integration of <scp>ZnS</scp> and Sulfurized Polyacrylonitrile Hybrid Anode Materials

High‐performance lithium‐ion batteries and sodium‐ion batteries have been developed utilizing a hybrid anode material composed of zinc sulfide/sulfurized polyacrylonitrile. The in situ‐ generated zinc sulfide nanoparticles serve as catalytic agents, significantly enhancing conductivity, shortening diffusion paths, and accelerating reaction kinetics. Simultaneously, the sulfurized polyacrylonitrile fibers form a three‐dimensional matrix that not only provides a continuous network for rapid electron transfer but also prevents zinc sulfide nanoparticle aggregation and mitigates volume changes during charge–discharge cycles. Moreover, the heterointerface structure at the junction of zinc sulfide nanoparticles and the sulfurized polyacrylonitrile matrix increases the availability of active sites and facilitates both ion adsorption and electron transfer. As an anode material for lithium‐ion batteries, the zinc sulfide/sulfurized polyacrylonitrile hybrid demonstrates a high reversible capacity of 1178 mAh g −1 after 100 cycles at a current density of 0.2 A g −1 , maintaining a capacity of 788 mAh g −1 after 200 cycles at 1 A g −1 . It also exhibits excellent sodium storage capabilities, retaining a capacity of 625 mAh g −1 after 150 cycles at 0.2 A g −1 . Furthermore, ex‐situ X‐ray photoelectron spectroscopy, X‐ray diffraction, 7 Li solid‐state magic angle spinning nuclear magnetic resonance, and in situ Raman are employed to investigate the reaction mechanisms of the zinc sulfide/sulfurized polyacrylonitrile hybrid anode, providing valuable insights that pave the way for the advancement of hybrid anode materials in lithium‐ion batteries and sodium‐ion batteries.