In this research, a new porous organic polymer based on triazine and cyclohexanone rings was synthesized via Schiff base condensation, and its performance as an adsorbent for the removal of Methyl Red dye from aqueous solution was investigated. The synthesized polymer was characterized by FT-IR, XRD, SEM, EDS, TEM, TGA, and BET analyses. Five important parameters of pH (4–10), contact time (10–120 min), adsorbent dose (5–10 mg), initial dye concentration (10–70 mg/L), and temperature (25–45 °C) were investigated to optimize the adsorption conditions. Solution pH of 4, contact time of 80 min, adsorbent dose of 8 mg, initial dye concentration of 50 mg/L, and temperature of 45 °C were obtained as the best conditions for the adsorption of methyl red dye. Two widely used Langmuir and Freundlich models were employed to investigate the adsorption isotherm, and the obtained data showed that the adsorption process follows the Langmuir isotherm with a correlation coefficient ( R2 = 0.9784) which indicates monolayer adsorption. The achieved maximum adsorption capacity was 178.57 mg/g. Also, the results of kinetic studies indicate that the adsorption process follows the pseudo-second-order kinetic, which suggests that chemical interactions play an important role in dye removal. Furthermore, the results showed that the adsorption process of methyl red dye by polymer is endothermic.