In the last few years, the construction of purely organicmolecule-based magnetic materials has become a topic of interest. [1] Since the first organic ferromagnet was discovered in 1991, [2] a number of other purely organic radicals exhibiting bulk ferromagnetic ordering at very low temperatures (generally below 1.5 K) have been found. [3] For this property to be achieved, synthetic tailoring of open-shell building blocks that allow both a proper control over their supramolecular assembly and the establishment of correct magnetic interactions, are required. Crystal engineering through hydrogenbonding interactions is a powerful method for achieving both conditions. From a structural point of view, the directional and often predictive nature of hydrogen bonds may allow control of the long-range supramolecular order in solid state. [4] Besides their structural control, hydrogen bonds have also been shown to favor magnetic exchange interactions between bound radical molecules of a-nitronyl nitroxides, a-imino nitroxide, or tert-butyl nitroxide derivatives. [5] For instance, attempts to control packing, and therefore magnetic ordering, in phenyl nitronyl aminoxyl radicals substituted by one or two OH groups have been carried out. [6] However, even though