The commercialization of lithium–sulfur batteries is limited by their low sulfur utilization rate and poor cycling stability. In this study, we successfully synthesized a nitrogen-doped porous aerogel material (GA/HNBRL) with high structural stability using graphene oxide (GO) as the carbon source and hydrogenated nitrile butadiene rubber latex (HNBRL) as a modifier. The synergistic effect of physical adsorption and chemical anchoring of GA/HNBRL carrier materials ensures high polysulfide adsorption and accelerated redox kinetics. Additionally, the incorporation of HNBRL enhances the mechanical properties of the carrier material, allowing for a higher sulfur loading and reducing the volume expansion of the active substance when used as a self-supporting material. The S@GA/HNBRL electrode material was prepared and could achieve an initial discharge specific capacity of 1315.6 mAh/g at a rate of 0.1 C without the involvement of current collectors, conductive agents, and binders. After 300 cycles at 0.1 C, its discharge specific capacity can still reach 870.9 mAh/g. In particular, the battery can still achieve a discharge specific capacity of 423.3 mAh/g after 500 cycles at a 1 C rate. This study provides a new approach for the application research of self-supporting materials in lithium–sulfur batteries by combining controllable porous structures with higher conductivity polymer materials.