Aluminosilicates are widely used as sorbent materials, ion exchangers, and catalysts. While they are often synthesized by hydrothermal methods, microorganisms may open “green” synthesis ways. Diatoms can incorporate aluminum into their micro- and nanostructured silica-based cell walls. Thus, diatoms create intricately structured aluminosilicate materials. The present study investigates not only possible morphological changes during the in vivo Al-enrichment of the diatom species Thalassiosira pseudonana, but also the increase of the specific surface area of Al-enriched biosilica in vitro by etching with alkaline solutions.