The contaminant dyes that, even at low concentrations, may cause a series of adverse effects in humans and animals, and their removal by adsorption methods using alternative adsorbents as natural fibers, are regarded as a research topic that has become increasingly relevant. In this study, corn straw (CS), an agro-industrial residue, was used to remove dyes. The samples were characterized by ATR-FTIR, SEM-EDS, zeta potential, diffuse spectra, and colorimetry, before and after dye removal. The analyses allowed us to differentiate the morphology of CS after the treatment’s fiber on the adsorbent surface. The zeta potential showed a negative surface charge, but the acidic or alkaline treatment affected the surface charge of the sample, influencing the adsorption of cationic or anionic dyes. Adsorption data presented an increased removal when alkaline treatment was applied for the methylene blue (MB; qmax = 16.7 mg g−1), and the acid treatment was more effective for the Congo red (CR; qmax = 2.13 mg g−1). After color stability tests, it was observed that the anionic dye CR was more easily desorbed due to the surface charge of the adsorbent. Due to the chemical treatment, corn straw proved to be a good sustainable adsorbent for removing anionic or cationic dyes from aqueous media, contributing directly to the objective of sustainable development (#6—drinking water and sanitation) and with SDG numbers 3, 11, 12, 14, and 17.