The synthesis, in one-pot, of an intimate composite material that simultaneously possesses ordered mesostructured MSU-S_BEA and well-defined zeolite Beta (*BEA) material over micron-scale domains is described. The synthesis is a simple solution-based two-step reaction that is a modification of the Al-MSU-S_BEA system and permits control of most physico-chemical aspects of both components of the composite material. The method appears to significantly improve the materials and catalytic properties of either of the individual components of the composite. Through manipulation of reaction alkalinity, Si/Al reagent ratio and crystallization time, control over the micropore/mesopore ratio, the SiO₂/Al₂O₃ ratio and the extent of crystallization can be achieved. While the composite material simultaneously exhibits highly ordered arrays of hexagonal mesopores and microporous zeolite Beta (*BEA), the particles tend to exhibit only the morphology of *BEA. The synthesis system also allows highly ordered pure end members of zeolite *BEA or hexagonal Al-MSU-S_BEA to be prepared. The structural properties of the material combine aspects of both micro- and mesostructure, while the catalytic properties reflect those of zeolite *BEA with improved diffusional characteristics of the mesostructure. The catalytic properties of the new material do not exactly match those of physical admixtures of Al-MSU-S_BEA and *BEA, thereby suggesting that the new material is more structurally and catalytically homogeneous than a simple mixture.