The present study reports on the development and testing of novel bleaching agents containing co-doped metaloxide nanoparticles (NP; 0%, 5%, 10% v/w) and hydrogen peroxide (HP, 0%, 6%, 15%, and 35%). Bovine blocks (n = 200, A = 36 mm2) were obtained and randomly distributed into experimental groups (n = 10/group). NPs were incorporated into gels before bleaching (3 sessions, 7 days apart, 30 min/session, irradiated with violet light-LT). Color changes (ΔE00, ΔWID), mineral content (CO32−, PO43−), and topography were assessed (spectrophotometer, ATR-FTIR, and AFM) before and after bleaching procedures (14 days). Metabolic status and three-dimensional components of non-disrupted Streptococcus mutans biofilms were investigated using a multimode reader and confocal microscopy. The results indicate that ΔE00 and ΔWID significantly increased with NPs’ concentrations and LT. The enamel’s mineral ratio was adversely impacted by HP, but alterations were less pronounced when using NP-containing gels. The enamel’s topography was not damaged by the bleaching protocols tested. The bioluminescence results show that bleaching protocols do not render latent antibacterial properties to enamel, and the confocal microscopy results demonstrate that the 3-dimensional distribution of the components was affected by the protocols. The proposed nanotechnology improved the bleaching efficacy of experimental materials independent of hydrogen peroxide or irradiation and did not adversely impact the enamel’s surface properties or its chemical content.