Laser-ablated Al atoms react with (CN)2 in excess argon during condensation at 4 K to produce AlNC, Al(NC)2, and Al(NC)3, which were computed (B3LYP) to be 27, 16, and 28 kJ/mol lower in energy, respectively, than their cyanide counterparts. Irradiation at 220-580 nm increased absorptions for the above molecules and the very stable Al(NC)4- anion. Annealing to 30, 35, and 40 K allowed for diffusion and reaction of trapped species and produced new bands for the Al(NC)1,2,3 dimers including a rhombic ring core (C)(AlN)2(C) with C's attached to the N's, a (NC)2Al(II)-Al(II)(NC)2 dimer with a computed Al-Al length of 2.557 Å, and the dibridged Al2(NC)6 molecule with a calculated D2 h structure and rhombic ring core like Al2H6. In contrast, the Al(NC)4- anion was destroyed on annealing presumably due to neutralization by Al+. B3LYP calculations also show that aluminum chlorides form the analogous molecules and dimers. In our search for possible new products, we calculated Al(NC)4 and found it to be a stable molecule, but it was not detected here.