MIL-101(Cr) is one of the most well-studied chromium-based metal–organic frameworks, which consists of metal chromium ion and terephthalic acid ligand. It has an ultra-high specific surface area, large pore size, good thermal/chemical/water stability, and contains unsaturated Lewis acid sites in its structure. Due to the physicochemical properties and structural characteristics, MIL-101(Cr) has a wide range of applications in aqueous phase adsorption, gas storage and separation, and catalysis. In this review, the latest synthesis of MIL-101(Cr) and its research progress in adsorption and catalysis are reviewed.