Hypothesis: Nanoparticles removal from seawage water is a health and environmental challenge, due to the increasing use of these materials of excellent colloidal stability. Herein we hypothesize to reach this objective through complex coacervation, a straightforward, low-cost process, normally accomplished with non-toxic and biodegradable macromolecules. Highly dense polymer-rich colloidal droplets (the coacervates) obtained from a reversible charge-driven phase separation, entrap suspended nanomaterials, allowing their settling and potential recovery. Experiments: In this work we apply this process to highly stable aqueous colloidal dispersions of different surface charge, size, type and state (solid or liquid). We systematically investigate the effects of the biopolymers excess and the nanomaterials concentration and charge on the encapsulation and sedimentation efficiency and rate. This strategy is also applied to real laboratory water-based wastes. Findings: Long-lasting colloidal suspensions are succesfully destabilized through coacervate formation, which ensures high nanomaterials encapsulation efficiencies (-85%), payloads and highly tranparent supernatants (%T-90%), within two hours. Lower polymer excess induces faster clearance and less sediments, while preserving effective nanomaterials removal. Preliminary experiments also validate the method for the clearance of real water residuals, making complex coacervation a promising scalable, lowcost and ecofriendly alternative to concentrate, separate or recover suspended micro/nanomaterials from aqueous sludges. (c) 2020 Elsevier Inc. All rights reserved.