A series of silica-coated micrometer-sized poly(methyl methacrylate) latex particles are prepared using a Stöber silica deposition protocol that employs tetraethyl orthosilicate (TEOS) as a soluble silica precursor. Given the relatively low specific surface area of the latex particles, silica deposition is best conducted at relatively high solids to ensure a sufficiently high surface area. Such conditions aid process intensification. Importantly, physical adsorption of chitosan onto the latex particles prior to silica deposition minimizes secondary nucleation and promotes the formation of silica shells: in the absence of chitosan, well-defined silica overlayers cannot be obtained. Thermogravimetry studies indicate that silica formation is complete within a few hours at 20 °C regardless of the presence or absence of chitosan. Kinetic data obtained using this technique suggest that the adsorbed chitosan chains promote surface deposition of silica onto the latex particles but do not catalyze its formation. Systematic variation of the TEOS/latex mass ratio enables the mean silica shell thickness to be tuned from 45 to 144 nm. Scanning electron microscopy (SEM) studies of silica-coated latex particles after calcination at 400 °C confirm the presence of hollow silica particles, which indicates the formation of relatively smooth (albeit brittle) silica shells under optimized conditions. Aqueous electrophoresis and X-ray photoelectron spectroscopy studies are also consistent with latex particles coated in a uniform silica overlayer. The silica deposition formulation reported herein is expected to be a useful generic strategy for the efficient coating of micrometer-sized particles at relatively high solids.