A post-synthetic modification strategy has been used to prepare three solid base catalysts, including Er(btc)(ED)075(H2O)0.25 (2, btc = 1,3,5-benzenetricarboxylates, ED = 1,2-ethanediamine), Er(btc)(PP)0.55(H20)0.45 (3, PP = piperazine), and Er(btc)(DABCO)0.15(H2O)0.85 (4, DABCO = 1,4- diazabicyclo[2.2.2]octane), by grafting three different diamines onto the coordinatively unsaturated Er(III) ions into the channels of the desolvated lanthanide metal-organic framework (Er(otc)). The resulting metal-organic frameworks were characterized by elemental analysis, thermogravimetric analysis, powder X-ray diffraction, and N2 adsorption. Based on its higher loading ratio of the diamine, as well as its greater stability and porosity, catalyst 2 exhibited higher catalytic activity and reusability than catalysts 3 and 4- for the Knoevenagel condensation reaction. The catalytic mechanism of 2 has also been investigated using size-selective catalysis tests.