Copper(II) reacts with monoethanolamine and with N-2-hydroxyethyl-ethylenediamine in methanol to yield the complexes Cu(NH 2CH 2CH 2OH)(SCN) 2 and Cu(NH 2CH 2CH 2NHCH 2CH 2OH)(SCN) 2, respectively, while reaction with triethanolamine yields Cu(N{CH 2CH 2OH} 2{CH 2CH 2O})SCN. Magnetic susceptibility data and vibrational spectral data for Cu(NH 2CH 2CH 2NHCH 2CH 2OH)(SCN) 2 are consistent with a square planar coordination about the copper with N-bonded thiocyanate ligands in a monomeric unit, while Cu(NH 2CH 2CH 2OH)-(SCN) 2 is thiocyanate bridged in an exchange-coupled dimeric formulation and Cu(N{CH 2CH 2OH} 2-{CH 2CH 2O})(SCN) is apparently an alkoxo-bridged chain polymer.