The crystal structures and magnetic properties of a series of isostructural magnetic compounds, M-II{N(CN)(2)}(2), where M = Cu (1), Ni (2), Co (3) and Fe (4) are presented. The dicyanamide bridges the metal ions in 1 - 4 to form infinite 3-D metal-organic frameworks with a rutile-type structure. Magnetic data for 1 obey the Curie-Weiss law (Theta = -2.1 K). 2 and 3 are ferromagnets with Curie temperatures (T-C) of 21 and 9 K; 4 is a canted antiferromagnet (T-N= 18.8 K). The coercive field of 4 is 17800 Oe, the largest observed for any metal-organic compound. The maximum energy product (BH) is the highest for 2 and is comparable to alloys of SmCo5. We attribute the large coercive field to a combination of single ion and particle shape anisotropies.