Starting from the perhydrogenated silafullerane [BuN][Cl@Si(SiH)H], treatment with BBr leads to partially and exhaustively brominated clusters, [BuN][Cl@Si(SiBrH)Br] (120 eq. BBr, room temperature, 30 min) and [BuN][Cl@Si(SiBr)Br] (300 eq. BBr, 130 °C, 3 d). Perbromination is accompanied by a massively increased steric strain on the cluster surface, which explains why our approach achieves regioselective derivatization of the Si framework when mild conditions are maintained. Partial Br/H exchange on [BuN][Cl@Si(SiBrH)Br] (30 eq. iBuAlH, room temperature, 16 h) affords [BuN][Cl@Si(SiH)Br].
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