Particle deposit morphologies that resulted from evaporating ink-jetted microdroplets were controlled by varying the ink compositions and concentrations. The ink was a well-dispersed aqueous dispersion of monodisperse silica microspheres. Silica particles suspended in the microdroplet undergo self-assembly upon the evaporation of the solvent. A ringlike deposit of the self-assembled silica particles was produced from the water-based ink, while a uniform two-dimensional monolayer with a well-ordered hexagonal structure was obtained from the mixed-solvent-based inks. Variations in the deposit patterns can be explained in terms of competing effects between the convective and Marangoni flows, which vary with the types of the high-boiling-point solvent added to the ink. The macroscopic shape and microstructure of the silica colloidal deposits were observed by SEM, AFM, and a confocal microscope.