In the current study, iron-loaded dead leaf ash (Fe-DLA) was used as a novel catalyst in the heterogeneous catalytic ozonation process (HCOP) for textile wastewater containing Reactive Black 5 (RB-5). The research demonstrates a significant boost in removal efficiency, reaching 98.76% with 1.0 g/min O3 and 0.5 g/L catalyst dose, by investigating key variables such as pH, ozone and catalyst doses, initial concentration, and the presence of scavengers in 1 L wastewater. The addition of tert-butyl alcohol (TBA) reduced RB-5 elimination, indicating the involvement of OH radicals. Catalyst reusability decreased slightly (2.05% in the second run; 4.35% in the third), which was attributed to iron leaching. A comparison of single ozonation (Fe-DLA) adsorption and catalytic ozonation processes (Fe-DLA/O3) revealed that the combined process improved dye degradation by 25%, with removal rates ranking as Fe-DLA adsorption O3 Fe-DLA/O3, with an impressive 76.44% COD removal. These results strongly support RB-5 removal using Fe-DLA and HCOP at a basic pH, highlighting the catalyst’s utility in practical wastewater treatment.