A "nano-net" superstratum strategy is developed to stabilize layer-by-layer (LbL) films that incorporate nanoparticles. The superstratum immobilizes silica, gold, or magnetic nanoparticles and at the same time is permeable to small molecules. Unlike most strategies to stabilize LbL multilayers reported in the literature, our strategy does not directly cross-link the nanoparticles and polymers in the adjacent layer, thus circumventing the tedious processes of (surface) modification of the nanoparticles or polymers. The unique advantage of our strategy is further employed in the preparation of a model functional device, where mesoporous silica nanoparticles are held in the composite multilayers with enhanced stabilities. A model drug, methylene blue, is then loaded in large amounts due to the porous structure of the silica particles, and could be released in a delayed manner up to 55 h.