The marine collagens are biocompatible and biodegradable materials that are considered as a biomimetic approach for tissue regeneration. This study evaluated the effect of daily consumption of marine collagen supplement drink on enamel white spot lesions (WSLs), comparing the results against Regenerate system and Sylc air abrasion methods. Fifty human enamel slabs were allocated into five groups (n = 10 per group): non-treated (sound); non-treated (WSLs, 8% methylcellulose gel with 0.1 M lactic acid (pH 4.6) at 37 °C for 21 days); and three treated surfaces with marine collagen; Regenerate system; and Sylc air abrasion. The treatment lasted for 28 days followed by four weeks’ storage in artificial saliva (pH = 7.0, 37 °C). Evaluations were conducted via micro-Raman Spectroscopy and Knoop microhardness at varying depths (50–200 μm), followed by morphological assessments using scanning electron microscopy (SEM). The marine collagen-treated surfaces demonstrated higher phosphate intensity and Knoop hardness values (KHN) compared to WSLs (p < 0.001) up to 150 μm depth, approaching that of sound enamel and other treated surfaces (p > 0.05). A significant positive correlation (p > 0.001) was recognized between the mineral content and corresponding KHN, particularly in the superficial layers. Notably, a compact layer of mineral-like structure was observed at the marine-treated surfaces covering the exposed lesion and enhancing surface integrity. These findings suggest that the use of marine collagen supplements can effectively enhance the mineral content and surface integrity of demineralized enamel surfaces up to a depth of 150 μm, presenting significant implications for dental health management.