The growing utilization of renewable and residual biomasses for environmental preservation and remediation are important goals to be pursued to minimize the environmental impact of human activities. In this paper, sodium alginate (derived from brown algae) was crosslinked using chitosan (mainly derived from the exoskeleton of crustaceans) in the presence of biowaste-derived substances isolated from green compost (BBS-GC), to produce hydrogels and dried films. The obtained materials were tested as adsorbents for wastewater remediation. To this purpose, gels were characterized using a multi-analytical approach and used as active substrates for the removal of three differently-charged molecules, chosen as model pollutants: crystal violet, rhodamine B, and orange II. The effectiveness of the gel formulations was demonstrated and attributed to the variety of active functionalities introduced by the different precursors, the structural factors and the peculiar physicochemical properties of the resulting materials.