Generally, incorporating functional groups into the inner surfaces of nanoporous metal-organic frameworks (MOFs) can substantially enhance their favourable properties. This concept led to the design and synthesis of an amino-functionalized ligand known as 2,4-di(2-amino-4,6-dicarboxylphenyl)-6-(2,4-dicarboxylphenyl)pyridine (H6TDP-NH2). Consequently, with the aid of H6TDP-NH2, we generated a robust heterometallic InIIIDyIIIorganic framework of {(Me2NH2)3[InDy2(TDP-NH2)2]center dot 5DMF center dot 4H2O}n (InDy-MOF), which was built on the exquisite combination of [In(III)(CO2)4] units and [Dy(III)2(CO2)8] SBUs and characterized by the excellent features such as nano-caged voids with amino-functionalized inner surface, enormous permanent porosity and extraordinary surface area. Due to the cooperative action of Lewis acid-base interactions such as amino groups, free oxygen atoms, open metal sites, and Npyridine atoms, InDy-MOF exhibits highly efficient catalytic activity on the cycloaddition of CO2 with epoxides under mild solvent-free conditions and Knoevenagel condensation of aldehydes and malononitrile. Therefore, these results confirmed that a resource-intensive and environmentfriendly integrated heterogeneous catalyst could be uncomplicatedly developed by introducing amino groups on existing organic ligands, especially which had been proven to be an efficient pillar in previously documented porous MOFs.