<p>Developing efficient heterogeneous Fenton-like materials is crucial for widespread implementation as it addresses technical challenges associated with conventional Fenton processes. These challenges include the need for large quantities of homogeneous catalysts and resulting secondary pollution from added catalytic species and their oxides. This paper describes the synthesis of a highly effective NiCuAl-HT compound. The compound serves as a Fenton-like catalyst when combined with H₂O₂ to oxidize organic contaminants in a simulated synthetic wastewater from oil refineries ‘SPRW’. The catalyst was calcined at different temperatures (180°C, 320°C, and 870°C) to evaluate and compare its performance with that of the non-calcined catalyst. Calcination of the NiCuAl-HT material, formed by achieving high supersaturation with the molar ratio R: (Ni²⁺+Cu²⁺)/Al³⁺ equal to 2.0 and the molar ratio Ni²⁺/Cu²⁺ equal to 1.0, leads to the formation of nanometric oxides. The non-calcined sample exhibited superior performance for SPRW oxidation, as revealed by comparative analysis. The NiCuAl-HT/H₂O₂ system achieved almost complete mineralization, as shown by TOC analysis, with a 65.24% removal efficiency after 90&#xa0;min, the other systems where the material is calcined at 380°C and 870°C, TOC removal was 47.80% and 06.67%, respectively, setting all parameters at: H₂O₂/COD: 5, m_cat: 0.4&#xa0;g L⁻¹, T: 60°C, and pH: pH_PZC. The efficiency of the catalytic reaction can be attributed to the layered structure of HT and the inclusion of hydroxyl groups on the brucite sheets. The catalytic reaction’s effectiveness may be attributed to the layered structure of the HT and the inclusion of hydroxyl groups on the brucite sheets.</p>