The Argyle diamond mine is the only known source of type IaB hydrogen- and nitrogen-rich diamonds colored gray to blue to violet. Twenty such diamonds were studied to investigate the relationships between their spectroscopic characteristics and color grades. The unusual color is the result of broad absorption bands centered at ~520–565 nm and 720–730 nm. A pronounced 551 nm band is superposed on the 520–565 nm feature. Spectral deconvolution of this feature suggests that it may be a composite, including H-related absorptions at ~545 and 563 nm and bands at 520–530 and 551 nm. The near- and mid-IR regions exhibit strong absorptions, including those related to H and N, many of which become more intense with increasing color saturation. The PL spectra exhibit peaks associated with nickel-related defects, which may play an important role in the coloration of the more violet diamonds in this group. H-rich gray-to-blue-to-violet diamonds, which are not known to be treated, can be readily separated from similar-hued diamonds that may be HPHT enhanced or synthetic.