Inorganic solids with porosity on the mesoscale possess a high internal surface area and a well-accessible pore system. Therefore, it is a relevant task to equip the surfaces of such materials with a maximum density of various organic functional groups. Among these functions it is the capability of coordinating to metal species as a ligand that is of extraordinary importance in many areas, for example, in catalysis. This paper describes how prominent ligands containing donor functions such as carboxylic, thio, chelating, or amine groups can be obtained in the form of nanoporous organosilica materials. The coordination of metal centers such as CoII, MnII, VIV, or PtIV is studied in detail. The magnetic properties of the corresponding materials and some applications in catalysis are reported. A quantitative determination of the surface density of donor atoms by distance measurements using EPR spectroscopy is shown.