A series of bis(trialkoxysilylmethyl)aryl compounds 1-17 {[(RO)(3)SiCH2](2)Ar, R = Me, Et, Pr, Bu, Ar = 1,4-C6H4; R = Et, Pr, Bu, Ar = 1,4-C6H2Me2-2,6; R = Et, Pr, Bu, Ar = 1,4-C6Me4-2,3,5,6; R = Et, Pr, Bu, Ar = 1,3-C6H4; R = Bu, Ar = 1,2-C6H4; R = Et, Pr, Bu, Ar = 9,10-C14H8} prepared from the related bis(trichlorosilylmethyl)aryl compounds and characterised by H-1, C-13 and Si-29 NMR and IR spectroscopy, and high resolution mass spectrometry. The X-ray crystal structures of two of the bis(trichlorosilylmethyl)aryl precursor compounds are reported. Organosilicate xerogels prepared from the precursors 2, 7 and 12 are discussed. These have been studied by a combination of solid state NMR spectroscopy, scanning electron microscopy (one case) and nitrogen sorption porosimetry and their properties compared with those of xerogels derived from related bis(trichlorosilylmethyl)arenes.