A magnetite chlorodeoxycellulose/ferroferric oxide (CDC@Fe3O4) heterogeneous photocatalyst was synthesised via treated and modified cotton in two steps. The designed nanocomposites were characterised by FTIR, TGA, XRD, SEM, and VSM analyses. The Fenton-photocatalytic decomposition efficiency of the synthesised magnetic catalyst was evaluated under visible sunlight using Methyl Orange (MO) as a model organic pollutant. The impacts of several degradation parameters, including the light source, catalyst load, irradiation temperature, oxidant dose, and pH of the dye aqueous solution and its corresponding concentration on the Fenton photodegradation performance, were methodically investigated. The (CDC@Fe3O4) heterogeneous catalyst showed a remarkable MO removal rate of 97.9% at 10 min under visible-light irradiation. (CDC@Fe3O4) nanomaterials were also used in a heterogeneous catalytic optimised protocol for a multicomponent reaction procedure to obtain nine tetra-substituted imidazole derivatives. The green protocol afforded imidazole derivatives in 30 min with good yields (91–97%) at room temperature and under ultrasound irradiation. Generally, a synthesised recyclable heterogeneous nano-catalyst is a good example and is suitable for wastewater treatment and organic synthesis.