Laser-ablated rhodium and iridium atoms are reacted with nitric oxide and the products are isolated in solid neon and argon. Neutral nitrosyl complexes Rh(NO)(1-3) and Lr(NO)(1-3) are the main products, and weaker bands due to RhNO+, IrNO+, NRhO, and NIrO are also observed. DFT calculations for these products using the BPW91 and B3LYP functionals determine frequencies with the same accuracy found for other metal nitrosyls and are a useful predictive tool. The stretching frequencies observed for the isolated nitrosyls are close to those for analogous nitrosyl species on rhodium and iridium surfaces, which will aid in interpreting vibrational data for surface species.