A zwitterionic construction has been synthesized that covalently links a trialkylsilylium cation and a weakly coordinating carborane anion in one neutral molecule (see X-ray structure; Si green, C gray, B orange, Cl red). The silylium character of this molecule is supported by DFT calculations (see LUMO),29Si CP/MAS NMR spectroscopy, and reactivity. Copyright 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.