In this study, Tarbiat Modares University-10/poly pyrrole (TMU-10/PPy), a water-stable metal–organic framework/polymer composite, was successfully fabricated and applied as adsorbent for removal of methyl red from contaminated water. The pyrrole obtained novel-structured TMU-10@PPy composite showed high efficiency in removing the methyl red. Several variables affecting the adsorption efficiency of methyl red, that is, pH, amount of adsorbent, contact times, and the salt additive, were investigated and optimized. The best working conditions were as follows: sample pH, 5; amount of sorbent, 4 mg; contact time, 9 min; salt additive, 2% (wt/vol). The maximum adsorption capacity of TMU-10@PPy toward methyl red was 101.01 mg/g. The adsorption kinetics and isotherms of TMU-10@PPy were consistent with a pseudo-second-order kinetic model and the Langmuir isotherm model. It was found that TMU-10@PPy exhibited excellent reusability and had the potential for treating dye-polluted wastewaters.