IRMOF-3 nano/microcrystals with controllable morphologies and sizes were successfully obtained by a simple solvothermal method. The shape evolution of IRMOF-3 crystals from cube to truncated cube, cuboctahedron, truncated octahedron and finally to octahedron was achieved by adjusting the amount of surfactant. The surfaces of the IRMOF-3 nano/microstructures are affected by the reaction temperature, and the nano/microparticles show shape-dependent sorption properties.