The rational design of organic-inorganic hybrids poses considerable challenges, but will yield considerable rewards in numerous technologies including separations, catalysis, sensing, and optical/magnetic materials. In the current work we will present results on a novel class of OMS-hybrids wherein the organic phase is grown directly off the inorganic substrate. Melamine-based dendrimers can be grown easily and in high yield off amine-functionalized SBA-15. A detailed characterization of the materials using porosimetry, microscopy, and spectroscopy will be presented. We will also show results demonstrating the flexibility of the chemistry by using a variety of amines as linkers in the dendrimers. This gives us considerable flexibility for modulating the hybrid porosity via dendrimer generation and linker, but also gives us control over the chemistry presented on the OMS surface in a simple and rational way. Results will also be presented demonstrating the ability to selectively sequester a variety of complexes using these hybrids. We will also report ongoing work demonstrating the ability to reversibly tether the dendrimer to the OMS surface using disulfide chemistry, and our preliminary efforts into using the melamine dendrimer-OMS hybrid as a scaffold for performing enantioselective organocatalysis with suitably functionalized dendrimers.