This feature article is a timely review of a portion of the authors' work concerning the chemistry of dendrimers and subsequent related fluorescent probes. The design of supramolecular systems provides an original approach to nanoscience and nanochemistry. The construction of well-defined functional architectures of nanometric size represents a way of performing programmed engineering of nanomaterials. Among the nanomaterials, dendrimers are set apart, and very recently a large number of works have been devoted to the elaboration of molecular sensors. These two aspects will be developed in this article from the authors' experience with calixarenes.