This chapter describes the state of the art of the synthesis, characterizat
ion, functionalization, and possible applications of all-phenylene dendrime
rs. Due to their high number of benzene rings, this type of dendrimer disti
nguishes itself by high stiffness, shape persistence, and nanometer dimensi
ons. This allows their use especially as chemically and thermally inert nan
o-supports for, e.g., chromophores, catalysts, but also as hosts for guest
molecules due to large stable cavities. In addition, the surface and bulk s
elf-organization properties of these polyphenylene dendrimers are presented
.