Layers of a layered double hydroxide, containing aluminum 4-fold coordinated, were partially folded in order to obtain a fibrous hydrotalcite-like compound. The hydrotalcite layers, in the presence of an anionic surfactant (sodium dodecyl sulfate) after hydrothermal treatment for 2 weeks, acquire a mesoporous-like arrangement. The transformation was monitored by techniques sensitive to structural and textural properties. Results suggest that brucite-like layers can be joined throughout unsaturated coordinated aluminum, that is, tetrahedral aluminum which links through hydrogen bonds to form aluminum octahedrally coordinated. The fractal dimension parameter was very sensitive to evolution from layered to fibrous hydrotalcites.