Positively charged contaminants can be strongly attracted by sulfanilic acid-functionalized graphene oxide. Here, sulfonated graphene oxide (GO-SO3H) was synthesized and characterized for cationic crystal violet (CV) adsorption. We further studied the effect of pH, initial concentration, and temperature on CV uptake. The highest CV uptake occurred at pH 8. A kinetic study was also carried out by applying the pseudo-first-order and pseudo-second-order models. The pseudo-second-order’s adsorption capacity (qe) value was much closer to the experimental qe (qeexp:0.13, qecal:0.12) than the pseudo-first-order model (qeexp:0.13, qecal:0.05). The adsorption performance was accomplished rapidly since the adsorption equilibrium was closely obtained within 30 min. Furthermore, the adsorption capacity was significantly increased from 42.85 to 79.23%. The maximum adsorption capacities of GO-SO3H where 97.65, 202.5, and 196.2 mg·g−1 for CV removal at 298, 308, and 328 K, respectively. The Langmuir and Freundlich adsorption isotherms were applied to the experimental data. The data fit well into Langmuir and Freundlich except at 298 K, where only Langmuir isotherm was most suitable. Thermodynamic studies established that the adsorption was spontaneous and endothermic. The adsorption mechanism was revealed by combining experimental and computational methods. These findings suggest that GO-SO3H is a highly adsorbent for removing harmful cationic dye from aqueous media.