Concept The last decade has seen growing attention in the synthesis and characterization of crystalline porous metal organic frameworks (MOFs) compounds in virtue of their potential applications in gas storage, separation and catalysis.[1] Among the different MOFs, the iron(III) 1,3,5-benzene tricarboxylate (Fe-BTC), well known as MIL-100(Fe), is one of most interesting 3D hybrid supertetrahedral structure that displays a hierarchy of microporous (ca. 5.5 and 8.6 Å) and mesoporous (ca. 25 and 29 Å).[2] The usually reported method for MOFs synthesis, including MIL-100(Fe), is the solvothermal one. Unfortunately, the solvothermal method imposes, already at the laboratory scale, hard reaction conditions, i.e. high temperature and pressure, use of large solvent amounts, and long synthesis times. Such reaction conditions would represent a serious drawback in the scale-up of the synthesis. Motivations and Objectives In this study we propose the Liquid-Assisted Grinding (LAG) [3] mechanosynthesis approach as an alternative route to synthesize a non-fluorinated Fe(BTC) sample with MIL-100(Fe) structure. Through this technique, high yields can be obtained in short reaction times working under mild conditions (room temperature, ambient pressure) using small solvent amounts mounts. The MFeLAG material, rapidly obtained by LAG, was characterized by XRDP, FTIR, SEM, TGA, N2 physisorption and adsorption microcalorimetry of NH3. For comparison, the features of a commercial Fe-BTC sample (Basolite F300) were investigated as well. The adsorption performance of the obtained MFeLAG sample for the removal of 4,6-dimethyldibenzothiophene (4,6-DMDBT) from 4,6DMDBT)/n-heptane solutions simulating a diesel fuel was also investigated. The stringent regulations on the sulfur content of fuels make adsorption technology an interesting, environmentally-friendly alternative to the conventional catalytic hydrodesulfurization processes [4]. Results and Discussion Liquid-assisted grinding is an effective strategy for the synthesis with quantitative yields of high quality iron(III) 1,3,5-benzene tricarboxylate (Fe-BTC) MOF of predominant crystalline cubic phase with good thermal stability, high surface area and pore volume. In comparison, the structural and textural features of commercial Basolite F300 appear rather poor. Both MFeLAG and the commercial sample have a quite high concentration of acid sites, as determined by ammonia adsorption calorimetry, with more pronounced heterogeneity of the sites in the case of Basolite F300. The MFeLAG sample performs much better than the commercial one in the ambient temperature adsorption of 4,6-DMDBT from a simulated low-sulfur diesel fuel.[5]