Abstract: | The complex (2,2′‐biquinoline‐κ2N,N′)(carbamoylcyanonitrosomethanide‐κ2N,O)chloridocopper(II) acetonitrile monosolvate, [Cu(C3H2N3O2)Cl(C18H12N2)]·CH3CN or [Cu(ccnm)Cl(biq)]·acn (acn is acetonitrile, biq is 2,2′‐biquinoline and ccnm is carbamoylcyanonitrosomethanide), (I), was prepared as a result of nucleophilic addition of water to the dicyanonitrosomethanide ion in the presence of CuII and biq. IR spectroscopy confirmed the presence of ccnm, biq and acn in (I). The solid‐state structure consists of the neutral complex containing ccnm and biq ligands, coordinated to the CuII atom in a bidendate chelating manner, and a chloride ligand, resulting in a distorted tetragonal pyramidal coordination of CuII. The asymmetric unit is supplemented by one molecule of solvated acn which, along with the nitrile group of ccnm, serves as an acceptor in intermolecular hydrogen bonding, creating infinite chains along the b axis. Magnetic measurements revealed a paramagnetic behaviour with a very small Weiss temperature Θ = −0.32 K and high anisotropy of the g tensor (gx = 2.036, gy = 2.120 and gz = 2.205). |