The reaction of bis(silylenyl)‐substituted ferrocene 1 with two molar equivalents of BPh3 yields the corresponding bis(silylene–borane) Lewis adduct 2. The latter is capable to activate CO2 to furnish the borane‐stabilized bis(silanone) 3 through mono‐oxygenation of the dative SiII→B silicon centers under release of CO. Removal of BPh3 from 3 with PMe3 affords the corresponding 1,3,2,4‐cyclodisiloxane and the Me3P−BPh3 adduct. All isolated new compounds were characterized and their molecular structures were determined by single‐crystal X‐ray diffraction analyses.