Colloidal silica microspheres of 0.5 and 1 micron were deposited into thin films on a glass substrate via a rapid convective deposition method. By varying deposition rate and contact angle, the optimal operating ranges in which 2D closed-pack of silica existed were obtained. Using a confocal laser scanning microscope, dynamic self assembly of colloidal particles under capillary force during solvent evaporation was revealed. In addition, interaction between substrate and colloidal particles played an important role in formation of ordered crystalline arrays. The interaction was altered by varying pH (2-11) and salt concentration of either substrate rinsing solution or colloidal suspension. Using the same technique, stacked layers of 1 micron silica monolayer on top of 1.1 micron polystyrene monolayers and subsequent melting of the polystyrene to partially wet the silica microspheres were deposited on GaN layer. This process was implemented on the top p-GaN layer of InGaN quantum wells light emitting diode (LEDs) device structure, resulting in the formation of a microlens array for enhancing its light extraction efficiency. This approach led to ~230% increase of the LEDs output power.