In this paper, we report the synthesis and characterization of a novel hybrid with an inorganic-organic structure formulated as [[Nd2(L(1))2(L(2))(H2O)7][H2SiW12O40]]n·4H2O (1), in which HL(1) = nicotinic acid and H2L(2) = 2-hydroxynicotinic acid. Interestingly, L(1) and L(2) are generated from an in situ transformation of the original ligand, pyridine-2,3-dicarboxylic acid under hydrothermal conditions. Structural analysis showed that this compound is a one-dimensional linear coordination polymer constructed from a repetition of the Keggin anion as a bidentate bridging ligand and one propeller-like dinuclear neodymium complex. Furthermore, in the packing arrangement, hydrogen bonds and anion-π interactions connect the adjacent chains to extend the structure into a 3D architecture. The magnetic properties of this compound have also been studied by measuring its magnetic susceptibility in the temperature range 1.8-300 K. We also analyzed the coordination ability of the SiW12 Keggin anion in the reported structures up to now. Finally, we have performed a DFT computational study on the noncovalent anion-π interactions between the Keggin anion and the aromatic ligands coordinated to Nd.