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An abundant hollow nanostructure is crucial for fast Li⁺ and K⁺ diffusion paths and sufficient electrolyte penetration, which creates a highly conductive network for ionic and electronic transport. In this study, we successfully developed a molecular-bridge-linked, organic–inorganic hybrid interface that enables the preparation of in situ nitrogen-doped hollow carbon nanospheres. Moreover, the prepared HCNSs, with high nitrogen content of up to 10.4%, feature homogeneous and regular morphologies. The resulting HCNSs exhibit excellent lithium and potassium storage properties when used as electrode materials. Specifically, the HCNS-800 electrode demonstrates a stable reversible discharge capacity of 642 mA h g⁻¹ at 1000 mA g⁻¹ after 500 cycles for LIBs. Similarly, the electrode maintains a discharge capacity of 205 mA h g⁻¹ at 100 mA g⁻¹ after 500 cycles for KIBs. Moreover, when coupled with a high-mass-loading LiFePO₄ cathode to design full cells, the HCNS-800‖LiFePO₄ cells provide a specific discharge capacity of 139 mA h g⁻¹ at 0.1 C. These results indicate that the HCNS electrode has promising potential for use in high-energy and environmentally sustainable lithium-based and potassium-based batteries.