This research seeks to optimize Nd:YAG laser cleaning parameters for the removal of corrosion products on historic iron alloy surfaces. This article presents the treatment of a 19th-century, European scale armor jazeran in the collection of the Arms and Armor Department at The Metropolitan Museum of Art. Laser cleaning was coupled with traditional mechanical cleaning techniques to increase the time efficiency of treatment while best preserving the composite material construction of the artifact and the aesthetic expectations of treatment. Laser cleaning using an 8 ns, Q-switched, Nd:YAG laser at 532 nm was found more effective at corrosion removal and less damaging to the underlying metal surface than laser cleaning at 1064 nm. Wavelength-dependent absorption and scattering effects on the laser cleaning of the corroded iron alloy surfaces were investigated. The composition, morphology, and stratigraphy of the corrosion layers were characterized and the effects of laser cleaning of these corrosion layers at 1064 nm and 532 nm were examined using stereomicroscopy, scanning electron microscopy -energy dispersive spectroscopy and back-scattered and secondary electron imaging, Raman spectroscopy, Fourier transform -infrared spectroscopy, and thermally assisted hydrolysis and methylation -gas chromatography -mass spectrometry. It was found that the success of the 532 nm laser cleaning is consistent with the green laser's more resonant energy absorption and decreased scattering length as compared to 1064 nm. These data were used to optimize the optical parameters of the laser energy interaction with the corrosion products to develop more effective and safer laser cleaning profiles for the removal of ferrous corrosion layers on the historic iron alloy surface.