This study presents a novel strategy to enhance the performance of lithium-sulfur (Li-S) batteries by using a lightweight, three-dimensional (3D) nitrogen/sulfur (N/S) codoped graphene sponge as an electrode material. The N/S codoped graphene sponge provides a high sulfur loading, facilitates fast charge transfer, and improves the immobilization of polysulfide ions. The hetero-doped N/S sites exhibit strong binding energy and effectively anchor polysulfides, leading to a high specific capacity of 1,200 mAh g−1 at 0.2C rate, a high-rate capacity of 430 mAh g−1 at 2C rate, and excellent cycling stability with a capacity decay of only 0.078% per cycle over 500 cycles. The graphene sponge's interconnected network enhances electron and ion transport, while the N/S doping increases the affinity between polysulfides and the carbon framework. This approach demonstrates the potential of using 3D current collectors and surface chemical modifications to achieve high-energy density and long-life energy storage devices.This study presents a novel strategy to enhance the performance of lithium-sulfur (Li-S) batteries by using a lightweight, three-dimensional (3D) nitrogen/sulfur (N/S) codoped graphene sponge as an electrode material. The N/S codoped graphene sponge provides a high sulfur loading, facilitates fast charge transfer, and improves the immobilization of polysulfide ions. The hetero-doped N/S sites exhibit strong binding energy and effectively anchor polysulfides, leading to a high specific capacity of 1,200 mAh g−1 at 0.2C rate, a high-rate capacity of 430 mAh g−1 at 2C rate, and excellent cycling stability with a capacity decay of only 0.078% per cycle over 500 cycles. The graphene sponge's interconnected network enhances electron and ion transport, while the N/S doping increases the affinity between polysulfides and the carbon framework. This approach demonstrates the potential of using 3D current collectors and surface chemical modifications to achieve high-energy density and long-life energy storage devices.