In recent decades, carbon dioxide (CO2) have become a serious threat in environment inspect, which was known as the main factor for the green-house effect. However, conventional methods of the utilization of CO2, for example, decreasing the CO2 level in the atmosphere through using chemical synthesis to produce functional chemicals or fuels concurrently. Traditionally, the effective routes to harvest CO2 is thermal energy activation via using higher reaction temperature or gas pressure, which can make this reaction difficult to industrialize. More attractive and green strategies for the utilization of CO2 is photocatalytic or electrocatalysis. About the above aspects, photocatalysis is one of the most effective and clean routes, wide application and perspective of pollution degradation and hydrogen evolutions. Remarkable efforts have been directed towards achieving efficient CO2 activating with photocatalysts by using wide-bandgap semiconductors, such as TiO2, SrTiO3, ZnO, SiC, ZnS, etc . Besides, the heterogeneous include metal-organic frameworks (MOFs) in addition to the oxide semiconductors such as MIL-101, ZIF-8 and UiO-66 have been recently employed as photocatalysts , since the modifcation of the coordination chemistry, energy bandgap, organic ligands, and composition of metal clusters can regulate light absorption and charge separation. It is known that MIL(125)-NH2 (Ti) has a preferable photocatalytic effect upon light excitation, which was consisted of titanium clusters coordinated to the organic linkers, i.e., 2-aminoterephthalic acid. Since previous studies have revealed that the applications of MIL(125)-NH2 (Ti) in photocatalytic CO2 reduction, while utilizing CO2 as a feedstock to produce small molecule chemicals, such as CO, CH4, HCOOH and CH3OH. However, there is still no report on the CO2 associated selective photocatalytic N-methylation of amines over MOFs.