With the development of industry, organic dyes used in printing, textile, plastic, foods, and cosmetics have brought health and environmental issues. A C2-symmetric benzene-based hydrogel with unique layered structure mimicking activated carbon was developed and found capable of the controllable adsorption of 97–99% of certain organic dyes (methylene blue and methyl violet 2B) within two minutes. The adsorption equilibrium of the dyes is in good agreement with the Langmuir adsorption isotherm model. The controllable adsorption of the dyes was confirmed by varying the pH of the medium. The hydrogel's rapid, highly effective, reusable, and controllable adsorption of organic dyes makes it possible to not only adsorb toxic dyes from wastewater, but also be used as potential delivery vehicles for small drug molecules in the field of drug delivery.