As of yet, unexamined aluminum bearing molecules may help elucidate aluminum chemistry and associated refractory atom reactions in the interstellar medium. The flexibility of modern quantum chemistry in the construction and analysis of novel molecules makes it perfectly suited to analyze molecules of astrochemical significance. In this paper, high level ab initio electronic structure calculations using the coupled cluster CCSD(T) and explicitly correlated coupled cluster CCSD(T)-F12 methods with large basis sets extrapolated to the complete basis set limit have been performed on the various [Al,N,C,O] isomers. The anharmonic rotational and vibrational spectroscopic parameters for all isomers are produced with these same levels of theory via quartic force fields and vibrational perturbation theory in order to aid in their potential laboratory or even astrophysical identification. The most stable isomer is determined here to be the aluminum isocyanate radical with linear equilibrium geometry AlNCO (X1Σ+). The NCO antisymmetric stretch of AlNCO has an intensity of 1500 km/mol, which should greatly aid in its infrared detection in the region around 2305 cm-1. Additionally, the AlOCN isomer is relatively low lying, possesses a 5.12 D dipole moment, and has a notable kinetic stability, making it a viable candidate for astronomical observation. All isomers are characterized by small frequencies, which indicates that these are floppy molecules. Isomers with a terminal aluminum atom are especially floppy, with bending modes less than 100 cm-1.