Synthetic dyes are persistent organic environmental pollutants that can cause extensive damage to living beings and to the ecosystem as a whole. Cost-effective, sustainable, and efficient strategies to deal with this type of pollution are necessary as it commonly resists conventional water treatment methods. Silver nanoparticles (AgNPs) synthesized using the aqueous extract from the leaves, stem, and fruits of Leucaena leucocephala (Leucena) were produced and characterized through UV–vis, TEM, EDS, SDL, XPS, XRD, and zeta potential, and they proved to be able to promote adsorption to remediate methylene blue and tartrazine pollution in water. The nanoremediation was performed and did not require direct exposure to sunlight or any special lamp or a specific reduction agent. The AgNPs produced using the extract from the leaves exhibited the best performance in nanoremediation and also presented antioxidant activity that surpassed the one from butylated hydroxytoluene (BHT). Consequently, it is an interesting nanotool to use in dye nanoremediation and/or as an antioxidant nanostructure.