Nitrophenols are persistent organic pollutants that pose serious environmental and health risks due to their toxic and lipophilic nature. Their persistence arises from strong aromatic stability and resistance to biodegradation, while their lipophilicity facilitates bioaccumulation, exacerbating ecological and human health concerns. To address this challenge, this study focuses on the synthesis and characterization of two different types of hybrid multi-core magnetic catalysts: (i) cobalt ferrite (Co-Fe2O4), which exhibits ferrimagnetic properties, and (ii) magnetite (Fe3O4), which demonstrates close superparamagnetic behavior and is coated with a novel and less hazardous phloroglucinol–glyoxal-derived resin. This approach aims to enhance catalytic efficiency while reducing the environmental impact, offering a sustainable solution for the degradation of nitrophenols in aqueous matrices. Transmission electron microscopy (TEM) images revealed the formation of a multi-core shell structure, with carbon layer sizes of 6.6 ± 0.7 nm for cobalt ferrite and 4.2 ± 0.2 nm for magnetite. The catalysts were designed to enhance the stability and performance in catalytic wet peroxide oxidation (CWPO) processes using sol–gel and solution combustion synthesis methods, respectively. In experiments of single-component degradation, the carbon-coated cobalt ferrite (CoFe@C) catalyst achieved 90% removal of 2-nitrophenol (2-NP) and 96% of 4-nitrophenol (4-NP), while carbon-coated magnetite (Fe3O4@C) demonstrated similar efficiency, with 86% removal of 2-NP and 94% of 4-NP. In the multi-component system, CoFe@C exhibited the highest catalytic activity, reaching 96% removal of 2-NP, 99% of 4-NP, and 91% decomposition of H2O2. No leaching of iron was detected in the coated catalysts, whereas the uncoated materials exhibited similar and significant leaching (CoFe: 5.66 mg/L, Fe3O4: 12 mg/L) in the single- and multi-component system. This study underscores the potential of hybrid magnetic catalysts for sustainable environmental remediation, demonstrating a dual-function mechanism that enhances catalytic activity and structural stability.
