The activity of two bifunctional metal-organic frameworks (MOFs) with IRMOF-9 topology that contain amino, phosphine oxide and methyl groups is described. The amino group acts as an active site for the Knoevenagel condensation of ortho, meta or para nitrobenzaldehyde and malononitrile, while the non-active site diphenylphosphoryl or methyl group moderate the spatial characteristics inside the MOF pores. The functional groups induce a unique catalytic response. The reaction activity was enhanced when catalysed by MOFs comparing with aniline, whereas the phosphine oxide retards formation of the ortho isomer product.