The organization of organic molecules and ions is an important area of supramolecular chemistry, where the control of molecular assemblies shows promise for generating materials with practical importance. In the process of designing new supramolecular motifs with various modes of organization, we have explored the strong electron donating ability of the tricyanomethanide anion (TCM). Although investigations of TCM exist in the literature, few provide insight into the structural tendencies of this molecular anion. Since TCM is a good electron donor, we anticipated the facile generation of salts using various organic cations. From our studies we observed that recrystallization of tricyanomethanide and either paraquat (N,N'-dimethyl-4,4'-bipyridinium) or 1,1'-bis(benzyl)-4,4'-bipyridinium formed cocrystalline salts in space groups P21/c and P-1, respectively. Inspection of the packing patterns of these molecular salts reveals TCM as a significant contributor to the supramolecular organization of these materials via notable intermolecular C-H•••N contacts and pi-stacking.