This study evaluated the effect of light-emitting diode (LED) illumination bleaching technique on the surface nanohardness of various computer-aided design and computer-aided manufacturing (CAD/CAM) ceramic materials. Twenty disk-shaped samples (width, length, and thickness = 10, 15, and 2 mm) were prepared from each of the ceramic materials for CAD/CAM, including Lava™ Ultimate (LV), Vita Enamic® (En) IPS e.max® CAD (Me), inCoris® TZI (IC), and Prettau® zirconia (Pr). The samples from each type of ceramic were randomly divided into two groups based on the different bleaching techniques to be used on them, using 35% hydrogen peroxide with and without LED illumination. The ceramic disk samples were bleached according to the manufacturer's instruction. Surface hardness test was performed before and after bleaching using nanohardness tester with a Berkovich diamond indenter. The respective Vickers hardness number upon no bleaching and bleaching without or with LED illumination [mean ± standard deviation (SD)] for each type of ceramic were as follows: 102.52 ± 2.09, 101.04 ± 1.18, and 98.17 ± 1.15 for LV groups; 274.96 ± 5.41, 271.29 ± 5.94, and 268.20 ± 7.02 for En groups; 640.74 ± 31.02, 631.70 ± 22.38, and 582.32 ± 33.88 for Me groups; 1,442.09 ± 35.07, 1,431.32 ± 28.80, and 1,336.51 ± 34.03 for IC groups; and 1,383.82 ± 33.87, 1,343.51 ± 38.75, and 1,295.96 ± 31.29 for Pr groups. The results indicated surface hardness reduction following the bleaching procedure of varying degrees for different ceramic materials. Analysis of variance (ANOVA) revealed a significant reduction in surface hardness due to the effect of bleaching technique, ceramic material, and the interaction between bleaching technique and ceramic material (p < 0.05). Bleaching resulted in a diminution of the surface hardness of dental ceramic for CAD/CAM. Using 35% hydrogen peroxide bleaching agent with LED illumination exhibited more reduction in surface hardness of dental ceramic than what was observed without LED illumination. Clinicians should consider protection of the existing restoration while bleaching.