In this study, opal–magnetite photocatalysts based on SiO₂ artificial opal crystals infiltrated with different concentrations of Fe₃O₄ nanoparticles (NPs) were synthesized using a combination of lateral infiltration and co-assembly methods. By adjusting the concentration of Fe₃O₄ NPs in the SiO₂ opal crystal, the energy band gap (Eg) was tuned to enable efficient degradation of methylene blue (MB) under visible light (410 nm and 575 nm). The photocatalytic process involved two stages: MB adsorption on the surface due to charge differences in the composite film and subsequent degradation through oxidative radicals on the catalyst’s surface. The developed material exhibited potential for applications in water remediation.