A series of transition metal NixCo1-x(N(CN)(2))(2) dicyanamide molecular magnet, 0 <= x <= 1, was chemically synthesized. Structure and magnetic properties were investigated by IR spectroscopy, neutron powder diffraction and temperature-dependent magnetization measurement. The neutron powder diffraction measurement established that all samples showed the rutile structure with Pnnm space group. The detailed Rietveld refinement results revealed a systematic decrease of unit-cell volume with increasing Ni content. We also observed a concurrent increase of the Curie temperature with Ni content due to the increase of superexchange interaction. (C) 2016 Elsevier B.V. All rights reserved.