“…Among efforts to acquire advanced molecule-based magnetic materials, rational molecular designs of component organic open shell entities have been crucial, and important attempts have been made. − Moreover, the more extensive the unpaired spin delocalization is, the larger will be the impact of substituent effects on the tuning of molecular electronic properties, underlain by exchange interactions in the crystalline state. , Recently, conjugated heavy atom heterocyclic radicals have been shown to be applicable as advanced conductive and magnetic materials as a consequence of easily tunable spin distributions and the ability to modify their crystal packing. ,, We note, however, that due to the persistence of such radicals and complicated synthetic procedures to obtain them, to date, the diversity of the hybrid organic radicals is rather poor. In this work, we have synthesized a series of stable all-organic hybrid nitroxides 1 (Figure ), in which phenoxyl is compactly π-conjugated, as new potential building blocks of advanced organic magnetic materials.…”