Nanostructured materials have drawn much attention due to their interesting physical property and high surface area. We have developed multifunctional nano-biocatalyst using various designed nanostrucutred materials. Hierarchically ordered mesocellular mesoporous silica materials (HMMS) were synthesized using a single structure-directing agent. To improve the retention of enzymes in HMMS, we adsorbed enzymes, and then employed crosslinking using glutaraldehyde (GA). The resulting crosslinked enzyme aggregates (CLEAs) show an impressive stability with extremely high enzyme loadings. Magnetically separable and highly active enzyme system was developed using nanostrucutred magnetic materials. Magnetically switchable bioelectrocatalytic system was constructed using magnetic mesocellular carbon foam (Mag-MCF-C) with ultra-large mesopores.