The amino group in the MOF NH 2 -MIL-101(Cr) was postsynthetically converted into urea-groups partially using either ethyl isocyanatoacetate, furfuryl isocyanate, p-toluenesulfonyl isocyanate or 3-(triethoxysilyl)propyl isocyanate in acetonitrile. The derived four novel urea-MOFs exhibit the expected lower BET surface areas and pore volumes than MIL-101(Cr) and NH 2 -MIL-101(Cr) MOFs but the partially p-toluenesulfonyl-ureamodified MOF exhibits an outstanding SO 2 adsorption capacity of 823 cm 3 g À 1 (corresponding to 36.7 mmol g À 1 or 70 wt.% at T = 0°C and 0.9 bar), which is the second highest SO 2 uptake of any known material today -surprisingly even better than for highly porous MIL-101(Cr) with an uptake of 645 cm 3 g À 1 SO 2 under the same conditions. The high uptake is linked to the favorable dipole interactions of SO 2 with the sulfonyl group of the p-toluenesulfonyl-modified MOF.