Nanotechnology is one of the most interesting areas concerned with consumer products including cosmetics, household appliances, electronics, textiles, and food production as well as in medical products. Environmentally benign, economical, practical, and efficient processes for the synthesis of graphene (rGO)-/graphene oxide (GO)-bounded metal nanoparticles and their use for the remediation of organic pollutants (dyes, pharmaceutical wastes, pesticides, etc.) have been increasingly important goals in the chemical community from economic, safety, and environmental points of view. In this chapter, various strategies have successfully demonstrated the synthesis of graphene-/graphene oxide-bounded metal nanoparticles using various natural sources (plant extracts, biomolecules, polysaccharide, alcohols, etc.) and their applications in environmental remediation.