<p>The management of sludge waste residue remains a critical environmental challenge, as improper disposal can contaminate major water bodies, disrupt aquatic ecosystems, and pose risks to human health. The sludge samples in river water and seawater exhibited distinct negative surface charges, as indicated by their zeta potential values, which strongly influence their stability and interaction with charged materials. In this work, a novel surface-active natural rubber latex (NRL) film was developed via optimized compounding and curing techniques to capture sludge particles through electrostatic and interfacial interactions. The formulation introduces intrinsic amphiphilic and protein-rich functionalities within the NRL matrix, enabling spontaneous adsorption of charged particulates without the need for external energy input. Fourier-transform infrared spectroscopy (FTIR) confirmed the presence of amine, protein, and peptide groups on the film surface after sludge interaction, validating the adsorption and surface entrapment mechanisms. The sludge removal efficiency was significantly enhanced in the presence of polyaluminum chloride (PACl), which served as a synergistic coagulant, enlarging sludge particle size and reducing zeta potential to promote aggregation and adhesion onto the NRL film. The combined NRL–PACl system demonstrates a novel, green, and reusable platform for passive sludge remediation, showing potential scalability for wastewater treatment in saline and freshwater environments.</p>