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The synthesis, structure, and three-dimensional lamellar array of a series of trans-bis(2-aminotroponato-κN,κO)palladium(II) complexes bearing linear alkyl chains (1a: n = 5; 1b: n = 8; 1c: n = 14; 1d: n = 16; 1e: n = 18, where n is the number of carbon atoms in the chain) attached to trans nitrogen donor atoms are described. The trans-coordination of the ligands, the cross-shaped molecular structures, and the crystal packing of 1b and 1c have been unequivocally established from single-crystal XRD studies. Highly regulated multilayered lamellar structures are observed for 1b and 1c, where every lamellar layer in the crystallographic ab plane, formed by π-stacking interactions of metal cores and van der Waals[a]