A new series of heterometallic lanthanide(III)-copper(I) coordination polymers Ln2(bdc)2(ina)2(H2O)2Cu x X (Hina = isonicotinic acid; H2bdc = 1,2-benzenedicarboxylic acid; Ln = Eu (1), Sm (2), Nd (3), X = ClO4-; Ln = Nd (4), X = Cl-) have been hydrothermally synthesized in the presence/absence of HClO4. Both compounds are isostructural and contained two distinct units of 2D Ln-bdc layers and linear [Cu(ina)2]-. The linear [Cu(ina)2]- complexes act as pillars and further link the Ln-bdc layers resulting in four heterometallic metal-organic frameworks, which represent the first pillared-layer 3d-4f framework with two distinct types of channels along the b and c axes. The compounds can be specified by the Schläfli symbol (47.63)(47.68) as a novel 3D (5,6)-connected net. Furthermore, the IR, TGA, PXRD, and UV-vis spectral and luminescent properties of 1-4 were also studied.