A monatomic zerovalent silicon(0) complex ("silylone") stabilized by the chelating bis(silylenyl)-ortho-carborane ligand, 1,2-(LSi)(2)-1,2-C2B10H10 [L = PhC(NtBu)(2)], has been synthesized from the redox reaction of the dipotassium bis(silylenyl)nido-carboranate salt, 1,2-(LSi)(2)-1,2-C2B10H10K2, and NHC-SiCl2 (NHC = {[HCN(2,6-iPr(2)C(6)H(3))](2)C:}). Markedly different from previous examples, this silylone undergoes reduction due to the closo-C2B10 cluster backbone, which is prone to accept up to two electrons to form the cage-opened dianionic nido-C2B10 cluster core. Surprisingly, the closo-C2B10 core of the silylone consumes only one molar equiv of potassium naphthalenide, in addition, one electron is intramolecularly transferred from the Si-0 atom to the C2B10 core to form an elusive bis(silylene)-stabilized Si-I radical cation which undergoes homocoupling to the corresponding isolable dicationic Si-I-Si-I complex.