This work presents the synthesis and characterization of a 3d-4f bimetallic complex based on the redox-active macrocyclic biquinazoline ligand, Mabiq. The mixed Yb-Ni complex, [(Cp*) 2 Yb(Mabiq)Ni]BArF (3), was synthesized upon reaction of [Ni II (Mabiq)]BArF (2) with Cp* 2 Yb II OEt 2 . The molecular structures of 3 and its sister complex, [(Cp*) 2 Yb(Mabiq)Ni][(Cp*) 2 Yb(OTf) 2 ] (1), confirmed the presence of a Yb(III) center and a reduced Ni-Mabiq unit. Spectroscopy (absorption and NMR), cyclic voltammetry and magnetic susceptibility studies were employed to analyze the electronic structure of 3, which is best described by the [(Cp*) 2 Yb III (Mabiq • )Ni II ] + formulation. Notably, the ligand centered radical is delocalized over both the diketiminate and bipyrimidine units of the Mabiq ligand. The magnetic susceptibility and variable temperature NMR studies for 3 denote coupling between the Ni-Mabiq site and the peripheral Yb center -previously unobserved in 3d-3d Mabiq complexes. The complex nature of the exchange interactions is highlighted by the multiconfigurational ground state for 3, comprising nearly degenerate singlet and triplet states.