LAUSR

Four heterobimetallic complexes (Ln = Ce (2), Gd (3), Tb (4), and Dy (5), H2L= Schiff base ligand) were synthesized from LNi (1) precursor (H2L = ligand N, N’‐bis(3‐methoxysalicylaldiimine)‐1,3‐propylene‐2‐ol). Compound 2, which crystallizes in the tetragonal system, differs from the other isostructural 3, 4, and 5 congeners which crystallize in the monoclinic system. The dc magnetic studies revealed ferromagnetic interaction between the Ni(II) (S = 1) and the lanthanide (Ln(III) = Gd, Tb and Dy) but not for Ce(III) in agreement with the computational results. The dynamic magnetic investigations highlighted field‐induced Single‐Molecule Magnet (SMM) behaviours for Ln(III) = Ce, Tb and Dy. In case of compound 4, it was determined that the slow magnetic relaxation occurred through an Orbach process only with D = 19.1(3) K and t0 = 3.99(4) × 10‐7 s (H = 1200 Oe). Electronic structures and magnetic properties have been investigated theoretically using Relativistic Density Functional Theory (DFT) calculations combined with the Broken Symmetry (BS) approach for the magnetic properties. Moreover, the computed Mayer and Nalewajski‐Mrozek (NM) Ni(II)‐Ob and Ob‐Ln(III) bond orders are found to be higher for 2 than for 3, 4, and 5, correlating well with the AF and Ferro character of each species.