We report the preparation, crystallization, and solid-state characterization of the first membersof a new family of spiro-bis-(1,9-diamino-substituted-phenalenyl)boron neutral radicals. The crystal structuresshow that the three radicals are monomeric and without close contacts in the crystal lattice. In all casesmagnetic susceptibility measurements confirm the presence of free radicals with one unpaired spin permolecule. Two of the new radical compounds are among the most highly conducting neutral organic solids,with room-temperature conductivities reaching
RT = 4 × 10
-2 S/cm. The measured conductivities correlatewith the closest intermolecular contacts in the solid state and with the calculated band dispersions, eventhough the bandwidths are much smaller than those found in other organic conductors.