Thermodynamic and spectrochemical data on the donor properties of dimethylcyanamide, (CHs)2NCN, toward chargetransfer types of acids, conventional Lewis acids, and nickel(II) are reported. Evidence from changes in the infrared and nmr spectra upon coordination is interpreted to indicate that the nitrile nitrogen is the donor atom. The C13-H coupling constants are very informative in elucidating the properties of this donor and the structure of these adducts. The donor properties of N,N-dimethylcyanamide are compared with those of acetonitrile and the differences are discussed. © 1968, American Chemical Society. All rights reserved.