Naturally occurring substances or polymeric biomolecules synthesized by living organisms during their entire life cycle are commonly defined as biopolymers. Different classifications of biopolymers have been proposed, focusing on their monomeric units, thus allowing them to be distinguished into three different classes with a huge diversity of secondary structures. Due to their ability to be easily manipulated and modified, their versatility, and their sustainability, biopolymers have been proposed in different fields of interest, starting from food, pharmaceutical, and biomedical industries, (i.e., as excipients, gelling agents, stabilizers, or thickeners). Furthermore, due to their sustainable and renewable features, their biodegradability, and their non-toxicity, biopolymers have also been proposed in wastewater treatment, in combination with different reinforcing materials (natural fibers, inorganic micro- or nano-sized fillers, antioxidants, and pigments) toward the development of novel composites with improved properties. On the other hand, the improper or illegal emission of untreated industrial, agricultural, and household wastewater containing a variety of organic and inorganic pollutants represents a great risk to aquatic systems, with a negative impact due to their high toxicity. Among the remediation techniques, adsorption is widely used and documented for its efficiency, intrinsic simplicity, and low cost. Biopolymers represent promising and challenging adsorbents for aquatic environments’ decontamination from organic and inorganic pollutants, allowing for protection of the environment and living organisms. This review summarizes the results obtained in recent years from the sustainable removal of contaminants by biopolymers, trying to identify open questions and future perspectives to overcome the present gaps and limitations.