Copper oxide and 3,3 ', 5,5'-biphenyltetracarboxylic acid are used as raw materials to obtain a MOF efficiently. At room temperature, we used water, ethanol and N, N-dimethylformamide (DMF) as liquid or vapors, respectively. The metal-organic framework-505 (MOF-505) was prepared by pre-ion and -liquid assisted grinding, then the Vapor-assisted aging (VAG) was carried out in different solvent vapor (water, methanol, DMF) to obtain the VAG-MOF-505. The results showed that VAG-MOF-505 with high crystallinity was obtained through pre-ion and -liquid assisted grinding with adding ethanol liquid (100 μL), then aged in ethanol vapor for 20 h at room temperature. By means of PXRD, FTIR, TGA, SEM, BET, structural characterization and pore analyses of the obtained product were performed. Its SEM and PXRD results showed that VAG-MOF-505 had high crystallinity similar to that made from the solvothermal method. Moreover, VAG-MOF-505 has a BET specific surface area of 1281 m2/g and an average pore diameter of 0.66 nm. This research result provides a new potential application of VAG method in green large-scale synthesis of MOFs.