Considerable attention has been focused on developing a synthetic route to a carbon-nitrogen material with mechanical and thermal properties comparable or superior to those of diamond. To date, no substance with the desired C3N4 stoichiometry in a silicon-nitride crystal lattice has been reported. One of the principal difficulties in the pursuit of ultrahard carbon-nitrogen (CN) solids is the characterization of amorphous CN samples. We describe a solid-state NMR study of a paracyanogen-like solid utilizing C-13-N-15 adiabatic-passage Hartmann-Hahn cross-polarization (APHH-CP) to perform dipolar filtering and show that this method is well-suited for recoupling C-13-N-15 in network solids. In addition, high-frequency electron paramagnetic resonance (EPR) indicates a density of electron spins of approximately 1 x 10(17) e(-)/cm(3). We conclude by discussing how NMR and EPR data may be useful for optimizing CN-polymer samples as potential precursors for ultrahard carbon nitrogen solids.