||A series of novel mono(imino)pyridine ligands with t -butyl, phenyl, and cyclohexyl substituents on the imino carbon atom have been synthesized by a new synthetic method. These ligands contain the imine functionality on the 2 position of the pyridine ring and either a hydrogen or a bromine on the 6 position of the pyridine ring. Certain ligands have been coordinated to NiBr 2 (DME) to create possible precatalysts for the polymerization of ethylene. The nickel(II) complexes have been studied by single crystal x-ray diffraction. A C 1 -symmetric bis(imino)pyridine ligand with a t -butyl substituent on one imino carbon and a phenyl substituent on the second imino carbon has also been synthesized using the new synthetic route. Extensive NMR studies have determined the bis(imino)pyridine ligand exists in two conformers.