We employed an electrophoretic deposition technique to prepare cylindrical colloidal crystals (CCCs) from polystyrene (PS) microspheres of 460 and 660 nm diameters using a carbon fiber (CF) with 7 μm diameter as the substrate. Measurements on the CCC diameter demonstrated growth rates that slowed down as time progressed. Scanning electron microscope images confirmed that the CCCs of 460 nm microspheres formed a face-centered cubic close-packed lattice, whereas an amorphous structure appeared for the CCCs of 660 nm. Subsequently, both CCCs underwent a potentiostatic electroplating to deposit Ni into the interstitial voids among the PS microspheres. After chemical removal of the PS microspheres, we fabricated cylindrical inverse opals (CIOs) in various diameters. As expected, better crystallinity was found on the CIOs of 460 nm microspheres as opposed to the 660 nm ones. The electrical resistivity for both CIOs exhibited a substantial reduction over that of the CF. Our CCCs and CIOs revealed considerable structure stability with excellent surface uniformity. The fabrication scheme enables rapid preparations of CCCs and CIOs in desirable lengths and diameters.