<p>Aqueous zinc-tellurium (Zn-Te) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of low utilization and severe volume expansion represents a significant obstacle to the development of aqueous Zn-Te batteries. Herein, a synergistic defect engineering and gradient pore structure strategy is proposed to construct tellurium nanoclusters/carbon composite cathode materials (DP-C/Te) for high-performance aqueous Zn-Te batteries. The gradient pore structure supplies confinement spaces that restrict crystalline tellurium formation, facilitating high-activity tellurium nanoclusters and enhancing structural stability. A defect-rich structure can accelerate the migration and aggregation of tellurium, not only leading to the formation of tellurium nanoclusters but also boosting the redox reaction of aqueous Zn-Te batteries. Additionally, robust C–O bonds can further facilitate the interfacial electron transfer. Consequently, the DP-C/Te cathode for aqueous zinc-tellurium batteries demonstrates sufficient specific capacity (481.75&#xa0;mAh g⁻¹ at 0.1&#xa0;A g⁻¹), superior rate performance (114&#xa0;mAh g⁻¹ even at 3&#xa0;A g⁻¹) and reliable cycling stability (81% capacity retention at 1&#xa0;A g⁻¹ after 1100 cycles). Furthermore, this work offers a promising perspective for high-performance aqueous Zn-Te batteries.</p> Graphical Abstract <p></p>