Different from the conventional method to construct pillared-layer metal-organic frameworks (MOFs) by using mixed bipyridyl and dicarboxylate ligands, herein, we present a new approach to build pillared-layer frameworks based on the pyridyldicarboxylate ligands which were predesigned with a certain shape. As exemplified, the ligands of 3(2',5'-dicarboxyphenyl)benzoic acid (H(3)dbba) and 3-(2',5'-dicarboxylphenyl)pyridine acid (H(2)dcpy) were selected and employed to construct three pillared-layer MOFs, [Zn-3(dbba)(2)(bipy)(DMF)].3DM.F center dot 4H(2)O (1) (bipy = 4,4'-bipyridine), and a pair of crystal polymorphs of [Zn(dCpy)]center dot 1.5DMF center dot 1.5H(2)O (2 and 3), under solvothermal reactions, respectively. In the structures of 1-3, the [Zn-2(COO)(4)] clusters are bridged by,the terephthalate units of dbba(3-)/dcpy(2-) to form 2D layers; these layers are further pillared by bipy and the benzoate units of dbba(3-) or the pyridine units of dcpy(2-) to furnish the 3D frameworks. All of them possess high porosity characterized by N-2 adsorption and exhibit high selective adsorption of C2H4 and CO2 over CH4.