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The operating parameters and resulting surface morphology of automated Langmuir–Blodgett deposition of monosized micrometer-scale silica colloids from an aqueous suspension are investigated. This apparatus allows continuous roll-to-roll deposition of particles into well-ordered arrays. The reproducible deposition of particle monolayers at low to moderate deposition rates at web speeds of less than 10 mm/s is possible and accurately characterized by a simple mass balance of particles deposited from solution. At faster deposition rates, Landau–Levich flow increases the film thickness such that flow instabilities hinder uniform particle deposition. A simple phase diagram outlines transitions from dispersed to multilayer coatings and from uniform to erratic deposition patterns. While the threshold of maximum deposition rate is well-defined for these conditions, changing operating parameters, particle size, and fluid …