Artificial opaline structure exhibits unique characteristics such as hexagonally-arranged pores and interconnected pore channels. Conventional fabrication routes involve gravitational and centrifugal sedimentation, as well as solvent evaporation of microspheres into an orderly colloidal template, followed by backfilling of materials into the interstitial voids among the closely-packed microspheres, and the selective removal of colloidal template. In this work, we adopt a sequential electrophoresis process in which a dc electrophoresis is used to direct the packing of polystyrene microspheres into a colloidal crystal with significantly-reduced crystallographic defects, followed by an ac electrophoresis to drive the oxide nanoparticles into the colloidal template. Relevant processing parameters are optimized and discussed. Structural observation and material characterization are performed using SEM, EDX, XRD, and XPS.