This paper reports a new way of modulating the strength of the Brønsted acid sites of a porous solid. Our approach consists of the grafting of various polar molecules (H 2 O, CD 3 OH, CF 3 CH 2 OH, and (CF 3 ) 2 CHOH) on MIL-100(Cr), a mesoporous crystallized chromium carboxylate with accessible unsaturated metal sites. We demonstrate, using infrared spectroscopy, that all these compounds do coordinate on the coordinatively unsaturated Cr 3+ sites. This generates controlled Brønsted acid sites whose strength, measured by CO adsorption at 100 K, depends on the nature of the adsorbate. It can vary from H 0 ) -3 (CD 3 OH) to -8 ((CF 3 ) 2 CHOH).