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The oxygen-bridged, silicon-substituted alkane Me3Si2CHSiMe22O 1 may be prepared by the reaction of Me3Si2CHLi with ClSiMe2OSiMe2Cl in refluxing THF. Similarly, the alkane Me3SiMe2MeOSiCHSiMe2CH222 is readily accessible from the reaction between Me3SiMe2MeOSiCHLi and ClSiMe2CH2CH2SiMe2Cl under the same conditions. Compound 1reacts with two equivalents of MeK to give the polymeric complex Me3Si2CSiMe22OK2OEt2∞5OEt2 after recrystallisation. Treatment of 2with two equivalents of either MeLi or MeK gives the corresponding complexes Me3SiMe2MeOSiCSiMe2CH22LiLiDME37DME3 and Me3SiMe2MeOSiCSiMe2CH22K2n8, respectively, after recrystallisation. Treatment of the alkane Me3Si2Me2MeOSiCH with one equivalent of MeK gives the polymeric complex Me3Si2Me2MeOSiCK∞3. These compounds have been identified by 1H and 13C1H NMR spectroscopy and elemental analyses and compounds 5OEt2, 7DME3and 3have been further characterised by X-ray crystallography. Compound 7DME3crystallises as a solvent-separated ion pair, whereas 5OEt2 and 3adopt polymeric structures in the solid state.