The reaction of Salen-like Zn II and Ni II precursors with carbacylamidophosphate lanthanide moieties yields six new types of 3d-4f compounds. The complexes were characterized by means of 1 H, 31 P NMR and IR spectroscopy, elemental analysis, ESI mass spectrometry, and X-ray diffraction analysis. Depending on the Schiff base ligands, the Ni II ion adopts either a square-planar or an octahedral geometry,[a] 3720 whereas the Zn II ion has a tetragonal-pyramidal geometry. The coordination number of lanthanides is nine or ten. Hydrolytic activities of some heterobimetallic Zn-Ln and Ni-Ln coordination compounds in the reaction of intramolecular hydrolytic degradation of the 2-(hydroxypropyl)-p-nitrophenyl phosphate were investigated. uclear complexes. [3][4][5][6] However, the investigations in the field of 3d-4f heterobinuclear compounds have mainly focused on their applications in magnetism and luminescence, [7][8][9][10][11][12][13][14][15] whereas their application in areas such as catalysis has, to our knowledge, not been reported.Recently, we have studied heteroleptic coordination compounds with β-diketone derivatives as carbacylamidophosphates (CAPh), containing the functional fragment C(O)-NHP(O). [16,17] Here, we report the synthesis, structural characterization, and catalytic properties of new binuclear 3d-4f complexes based on unsaturated lanthanide moieties with CAPh, and complexes of Zn II and Ni II with Schiff bases as additional ligands (Scheme 1). Scheme 1. Precursors for syntheses of 3d-4f complexes.