Layer silicates (phyllosilicates) are a well known source of nanolayers for technological applications (Auerbach et al. 2004). In particular, low-charge tetrahedraloctahedral-tetrahedral (TOT) layers of clay minerals, e.g. smectites, are used to prepare organoclay complexes, nanocomposites and pillared materials. This contribution aims to attract the attention on the possibility of using TOT-like layers of heterophyllosilicates (Ferraris et al. 1996) to prepare organoclay-like hybrids and pillared structures. The presence of five and six co-ordinated titanium in the layers of the heterophyllosilicates looks particularly appealing owing to the well known catalytic properties of this chemical element.