MOF-253 (Al(OH)(dcbpy), dcbpy = 2,2'-bipyr-idine-5,5'-dicarboxylic acid) obtained via a microwave-assisted synthesis was used for the construction of a supported Ru complex containing dcbpy (MOF-253-Ru(dcbpy)(2)) by coordi-nating its open N,N'-chelating sites with Ru(II) in Ru(dcbpy)(2)Cl-2. The as-obtained MOF-253-Ru(dcbpy)(2) acts as a bifunctional photocatalyst for simultaneous CO2 reduction to produce formic acid and CO, as well as semidehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to obtain 3,4-dihydroiso-quinoline (DHIQ). The performance over the surface-supported MOF-253-Ru(dcbpy)(2) is superior to that over Ru-doped MOF-253 (Ru-MOF-253) obtained via a mix-and-match strategy, indicating that the use of open coordination sites in the MOFs for direct construction of a surface-supported complex is a superior strategy to obtain an MOF-supported homogeneous complex. This study shows the possibility of using an MOF as a platform for the construction of multifunctional heterogeneous photocatalytic systems. The coupling of photocatalytic CO2 reduction with the highly selective dehydrogenation of organics provides an economical and green strategy in photocatalytic CO2 reduction and production of valuable organics simultaneously.