Re-use of the byproduct wastes resulting from different municipal and industrial activities in the reclamation of contaminated water is real application for green projects and sustainability concepts. In this direction, the synthesis of composite sorbent from the mixing of waterworks and sewage sludge coated with new nanoparticles named “siderite” (WSSS) is the novelty of this study. These particles can be precipitated from the iron(II) nitrate using waterworks sludge as alkaline agent and source of carbonate. Characterization tests using X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) mapping revealed that the coating process was correctly achieved and siderite nanoparticles were planted on the surface of the composite sorbent. Interaction between Congo Red dye and composite sorbent was evaluated through a set of batch tests under the variation of agitation time, pH of aqueous solution, and sorbent dosage. The results proved that the prepared sorbent had a high ability in the treatment of water contaminated with Congo Red dye in comparison with previous studies and the maximum adsorption capacity reached to maximum value i.e. 9416 mg/g. The sorption process was governed by electrostatic attractions; however, Sips and Pseudo-second-order models described this process with coefficient of determination greater than 0.99.