The presence of dyes in effluent poses various environmental as well as health hazards for many organisms. Although various remediation strategies have been implemented to reduce their effect, dyes still manage to infiltrate into the environment and hence new strategies are required to address some of the problems. This study investigated the innovation of two cationic water-soluble polymers viz., Proline-Epichlorohydrin-Ethylenediamine Polymer (PEP) and Thiazolidine-Epichlorohydrin-Ethylenediamine Polymer (TEP) that were used to remediate selected synthetic dyes from synthetic effluent by adsorption and dye reduction. Both polymers were synthesized using monomers of a secondary amine, epichlorohydrin and ethylenediamine and were subsequently characterized and modified and their remediation potential studied. In the first study, PEP was synthesized and characterized by 1H-NMR Spectroscopy, FT-IR Spectroscopy, dynamic light scattering, and thermogravimetric analysis (TGA). Thereafter PEP was modified with bentonite clay, by simple mixing of the reactants, to form a Proline-Epichlorohydrin-Ethylenediamine Polymer-bentonite composite (PRO-BEN); it was characterized by FT-IR Spectroscopy, scanning electron microscopy (SEM)/ energy dispersive X-ray spectroscopy (EDX), dynamic light scattering (DLS), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Adsorption studies were then undertaken with a synthetic effluent containing three textile dyes, viz., Reactive Blue 222 (RB 222), Reactive Red 195 (RR 195) and Reactive Yellow (RY 145). Various conditions were investigated including pH of the solution, temperature, sodium chloride concentration, initial dye concentration and the dosage of adsorbent used. The experimental data for all dyes followed a Langmuir isotherm. The adsorption process was found to be pseudo-second order. According to the thermodynamic parameters, the adsorption of the dyes was classified as physisorption and the reaction was spontaneous and exothermic. The data were also compared using studies with alumina as an adsorbent. Results showed that PRO-BEN exhibited better absorptivity and desorption than alumina making its use a better recyclable remediation strategy for the removal of organic dyes in wastewater treatment plants. In the second study, TEP was synthesized and then characterized by FT-IR Spectroscopy, 1H-NMR Spectroscopy, TGA and DLS. Thereafter, TEP was used to prepare TEP capped gold nanoparticles (TEP-AuNPs). Herein, two methods were investigated: the Turkevich method and an adaptation of the Turkevich method using bagasse extract. The TEP-AuNPs was characterized by FT-IR Spectroscopy, SEM, EDX, DLS and TEM. Thereafter the reduction of each of Allura Red, Congo Red and Methylene Blue was investigated with the TEP-AuNPs for its catalytic activity toward dye reduction. This study showed that the batch of AuNPs prepared by the Turkevich method had higher rates of dye reduction compared with AuNPs prepared using bagasse extract. Also the quantity of TEP used as capping agent greatly influenced the size, shape and surface charge of the nanoparticles as well as their catalytic performance: the Vroman effect explained this behavior of the TEP-AuNPs. It was finally concluded that whilst PRO-BEN, in the first study, showed excellent dye remediation properties, the second study on TEP-AuNPs showed good catalytic activity for the reduction of selected dyes, however, it was more effective at lower polymer concentration. Finally, both materials displayed good potential for the clean-up of selected synthetic dyes from synthetic effluents.