In recent decades, introducing messenger RNA (mRNA) into cells has garnered intense interest for diverse applications. Limited by the short half-life and cell-membrane impermeability of mRNA, the success requires delivery solutions. With extensive efforts devoted in the nanomaterials based mRNA delivery platform, current design strategies for mRNA delivery systems primarily focus on mRNA binding, intracellular delivery and protection from degradation, but few provide the functionality to directly regulate mRNA translation. Besides, current delivery technology has limited delivery efficiency in hard-to-transfect cells (e.g., macrophages). Thus, new strategies are highly desired to exploit the multifunctional nanoparticles as both transfection agents and translation regulators for enhanced mRNA delivery with improved performance.Inspired by our recent breakthroughs in mesoporous silica nanoparticles (MSNs) synthesis, combined with the fundamental regulatory mechanism and intracellular environment of specific cells, this thesis focuses on the synthesis of functional dendritic mesoporous silica nanoparticles (DMSNs) designed for enhanced mRNA delivery. A facile, water phase based synthetic system was developed for the fabrication of large pore DMSNs with controlled structure and composition. Through the systematic study of the structural evolution of dahlia-like DMSNs to pomegranate-like MSNs via a micelle filling mechanism, the heterogeneous porous structure of DMSNs was reported for the first time for delivery of two positively charged cargoes. By comparing tetrasulfide bond bridged dendritic mesoporous organosilica nanoparticles (DMONs) with inorganic DMSNs with keeping other parameters the same, the composition contribution on intracellular glutathione (GSH) depletion, translation pathway regulation and mRNA delivery performance in antigen presenting cells were studied for the first time.Moreover, zeolitic imidazolate framework-8 (ZIF-8) was introduced to grow inside the mesopores of DMONs. The combined effect of ZIF-8 and tetrasulfide bond on the intracellular regulation of GSH and mRNA delivery was studied, providing new understandings in controllable synthesis of advanced materials as mRNA delivery vehicles.In the first experimental chapter, we report a unique dynamic structural transition from large pore sized DMSNs with the dahlia-like morphology to pomegranate-like MSNs with small mesopores.The silica-coated micelle composites were revealed to contribute to the kinetic structural evolution and heterogeneity of DMSNs. The structural evolution window was finely controlled by several parameters, including reaction time, reaction temperature, molar ratio of anionic micelle penetration agents to cationic surfactant, type of anions and amount of silica precursor. The advantage of the heterogeneous DMSNs with dual mesopores was further demonstrated for the co-delivery of two positively charge molecules, ribonuclease (RNase A, pKa= 9.6, Mw = 13.7 kDa, a model therapeutic I acknowledge that copyright of all material...