Tooth bleaching is considered a non-invasive treatment, although the use of highly-concentrated products may provoke increased surface roughness and enamel demineralization, as well as postoperative sensitivity. Thus, the aim of this study was to investigate whether hydrogen peroxide (H2O2) concentration would affect tooth bleaching effectiveness and the enamel surface properties. Enamel/dentin bovine specimens (6 × 4 mm) were immersed in coffee solution for 7 days and evaluated with a spectrophotometer (Easyshade; baseline), using the CIEL*a*b* color parameters. Hardness was measured using a hardness tester. The specimens were randomly assigned into four groups: one negative control, in which the specimens were not bleached, but they were irradiated with a laser-light source (Whitening Lase II, DMC Equipments); and three groups using distinct H2O2 concentration, namely LP15% (15% Lase Peroxide Lite), LP25% (25% Lase Peroxide Sensy), and LP35% (35% Lase Peroxide Sensy), all products from DMC. The bleached specimens were also irradiated with the laser-light source. After bleaching, all specimens were evaluated using scanning electron microscopy (SEM). pH kinetics and rate was monitored during bleaching. The data were analyzed using ANOVA and Tukey’s test (p < 0.05). All bleaching gels produced similar color change (p > 0.05). Concerning hardness, only the LP25% and LP35% significantly reduced hardness after bleaching; also, there was a progressive tendency for a greater percentage reduction in hardness with increased H2O2 concentration of the gel (R2 = 0.9973, p < 0.001). SEM showed that LP25% and LP35% produced an etching pattern on enamel with prism rods exposure. In conclusion, H2O2 concentration above the 15% level does not increase bleaching effectiveness, and may increase the possibility for alteration of enamel hardness, surface morphology, and acidity of the medium. When using H2O2-based bleaching agents, dental practitioners should choose for less concentrated gels, e.g., around the 15% level.