Laser-ablated group 2 metal atoms exhibit different reactivities with (CN)(2) in excess argon and neon during condensation at 4 K. UV irradiation (220-290 nm) is required to activate Be to produce the linear CNBeNC di-isocyanide molecule with a strong antisymmetric C-N stretching band at 2104.3 cm(-1) and a C-N-Be-N-C stretching mode at 1265.7 cm(-1). The di-isocyanide appears at lower frequency and exhibits more nitrogen and less carbon isotopic shift than the cyanide counterpart, which is confirmed by B3LYP isotopic frequency calculations. Two weak bands were observed for the cyanide NCBeCN, and three absorptions were found for the mixed ligand CNBeCN molecule, which would be difficult to synthesize and put into a bottle. Mg reacts with (CN)(2) to form the CNMgNC counterpart at 2085.8 cm(-1) on annealing to 25 K. Absorptions for the Ca(NC)(2), Sr(NC)(2), and Ba(NC)(2) molecules at 2060.8, 2048.1, and 2045.9 cm(-1) increase on sample annealing with these more reactive heavier alkaline earth metal atoms, which have calculated twisted bowtie side-bound (CN) structures of C-2 symmetry with shorter computed M-N than M-C distances. NBO calculations for the latter molecules reveal natural charges of +1.54, 1.64, 1.71 e on the metal centers and -0.77, 0.82, and 0.855 e on the corresponding CN subunits, with a doubly occupied sp-sp o and two p-p pi bonds on each (CN), which supports an ionic model for bonding in these molecules. A weaker band at 2056.6 cm(-1) behaves nearly the same as the Ca bowtie band in the spectrum on 25 K annealing and photolysis, and it is assigned to the 6 kJ/mol higher-energy linear CNCaNC isomer. Additional similar sharp absorptions for a new Ca, Sr, and Ba reaction product at 2036.3, 2040.6, and 2036.0 cm(-1) increase on annealing at the expense of adjacent broader bands: B3LYP and NBO calculations validate their assignment to ionic hexagonal C-2h (MNC)(2) rings from the reaction of two M atoms with (CN)(2).