A complete understanding of the biological activity of nitric oxide (NO) is complicated by the different reactivity profiles of its various species and by the often complex decomposition behavior of the NO progenitors in common use. Here, we report that appropriately substituted C-nitroso compounds act solely as donors of neutral nitric oxide through a first- order homolytic C− N bond scission to release up to 88% nitric oxide in DMSO at 25° C. ...