MCM-41 type mesoporous silicate particles have attracted a significant amount of research interest due to the ordered porous structure of the materials, their facile synthetic methods, and their broad range of applications. [1][2][3][4] Further developments in the synthesis and modification of nanosized mesoporous silica materials have created new possibilities for biomedical applications. [5][6][7][8] As opposed to nonporous silica nanoparticles, both the surface and the pore interior of mesostructured nanoparticles can be modified with functional groups, such that they become compatible in various solutions and are able to store different types of molecules. [9][10][11][12][13][14][15] These nanomaterials have been well demonstrated for their biocompatibility, [16,17] and in their utilization as fluorescent markers for cells, [18] gene-transfection agents, [19] and delivery vehicles for proteins and anticancer drugs. [20,21] Studies of the interaction of mesoporous silicate nanoparticles with bacteria are rare. The nanoparticles were modified with dye molecules to enable studies of possible interaction using fluorescence microscopy. Rhodamine B isothiocyanate (RITC) was reacted with aminopropyltriethoxysilane and mixed with the silica precursor tetraethylorthosilicate (TEOS) to functionalize the interior pores and surface of the particles with the dye molecules without disrupting the mesostructure. [6,21,22] For our previous studies, two types of bacteria were used: Bacillus anthracis BH450 (B. anthracis), as the Gram-positive model, and Escherichia coli BL21 DE3 (E. coli), as the Gram-negative model. Upon mixing the nanoparticles with bacteria, red fluorescence of the nanoparticles was found to overlap with B. anthracis, but not with E. coli, suggesting that the particle adherence to the bacteria may depend on the bacterial strain and surface characteristic of the nanoparticles (Fig. S1, Supporting Information). Encouraged by these initial results and the report on use of nitric oxidereleasing silica nanoparticles as bactericidal agents, [23] we continued the studies in order to develop mesostructured silica nanocomposites that can store large amounts of antimicrobial materials and slowly release the bactericidal agents over an extended time period.The ability to encapsulate inorganic materials by growing mesostructured silica around them introduces additional functionality to the nanoparticles. Gold, semiconductor, and iron oxide nanocrystals can be incorporated within mesoporous silica nanoparticles to create a yolk/shell architecture without collapsing the mesostructure. [24][25][26][27] In comparison to the traditional coating of inorganic nanocrystals with nonporous silica or polymer, [28][29][30][31][32] the mesoporous silica shell offers the advantage of being able to store molecules or to slowly release the encapsulated inorganic materials. [33,34] Based on the works by Trewyn et al. in synthesizing mesoporous nanoparticles that release bactericidal cationic surfactants, [35] and Jiang et al. in prepar...