Anion redox reactions in layered cathode materials have attracted significant attention due to their remarkable potential to enhance the capacity and energy density of lithium-ion batteries. However, in conventional sulfide-based cathodes such as LixTiS2, anionic redox is only partially reversible at high voltages and suffers from rapid capacity fading. These challenges primarily originate from the intrinsic electronic band structure of LixTiS2, where the Ti3+/Ti4+ redox couple lies far above the S 3p band, suppressing ligand-to-metal charge transfer during Li+(de)intercalation. To overcome this limitation, we introduce a bandgap-engineering strategy via partial substitution of Ti3+ with Cr3+, effectively narrowing the d-p bandgap and activating sustainable sulfur redox chemistry. The Cr-substituted compound, Li0.80Cr0.67Ti0.33S2, exhibits sustainable sulfur redox activity, thereby achieving a higher capacity of 223.0 mA h g-1 and nearly doubling the energy density of pristine Li0.80TiS2. Furthermore, Li0.80Cr0.67Ti0.33S2 preserves its layered framework throughout the whole (de)lithiation process, indicating effective suppression of structural collapse during sulfur redox. Therefore, it demonstrates outstanding rate performance (77.5% capacity retention at 5.0C) and excellent long-term cycling stability (80% retention after 330 cycles), significantly outperforming its undoped counterpart. These findings highlight the critical role of ligand-metal d-p orbital overlap in enabling and stabilizing sustainable sulfur redox, providing valuable insights for the design of high-performance cathodes for next-generation lithium-ion batteries.