Dendrimers constitute an increasingly important field of research in chemistry for more than 15 years. After pioneering works concerning synthesis, the interest in dendrimers is now mainly driven by their properties and applications. This Account will emphasize the properties of a special class of dendrimers, that is, phosphorus-containing dendritic macromolecules, as tools for the elaboration of nanomaterials. Indeed, these dendrimers can be considered themselves as materials, or they can be used as an intrinsic constituent of a material or as a modifier of the surface of a material. In this latter case, a fundamental work about surfaces covalently modified by dendrimers recently opened the way to the elaboration of DNA chips.