Environmental pollution is one of the most challenging problems worldwide, and water is one of the most vulnerable environmental matrices, being an essential resource for life. The exponential increase in industrial manufacturing processes, technological development, urbanization, natural climatic events, and agricultural practices, among others, have generated environmental exposure to numerous chemical compounds that cause the contamination of aqueous matrices. This challenge has led to the development of hybrid nanocomposite biosorbents as an innovative strategy for the aqueous removal of relevant pollutants. These nanocomposites, created from biopolymeric hydrogels and nanoclays, are an effective, sustainable, and scalable strategy for the removal of these pollutants. Our work seeks to provide concrete solutions to the complex problems of water pollution, using the potential of nanocomposite biosorbents. The present work aims to develop materials with biosorbent capacities, based on natural and innocuous raw materials such as the biopolymers chitosan (Q) and sodium alginate (Alg), as well as natural and organomodified bentonite (B) and organomodified (OB) nanoclays. These starting materials are abundant, inexpensive, and environmentally friendly. Nanocomposite biosorbent hydrogels of Q/OB, Alg/B, and Alg/OB were developed using simple and low-cost techniques. The biosorbents were physicochemically and morphologically characterized. These tests revealed internal structures with large porosity, favorable for the diffusion and adsorption of the pollutant. Preliminary atrazine, ciprofloxacin, and arsenic removal tests were performed under batch conditions. The results showed promising biosorptions for all the pollutants studied. These results show the potential of the developed biohydrogels as efficient systems for the aqueous remediation of contaminants of relevance to mitigate a real problem of global concern.