Human molars were subjected to demineralization in acid gel followed by incubation in remineralization solutions without or with fluoride (1 or 1000 ppm). Photothermal radiometry (PTR) and modulated luminescence (LUM) frequency scans were performed prior to and during de/remineralization treatments. Transverse Micro-Radiography (TMR) analysis followed at treatment conclusion to determine mineral loss and lesion depth. The remineralization process illustrated a complex interplay between surface and subsurface mineral deposition, confining the thermal-wave centroid toward the dominating layer. Experimental amplitudes and phases were fitted to a coupled diffuse-photon-density-wave and thermal-wave theoretical model used to quantitatively evaluate evolving changes in thermal and optical properties of de/remineralized enamel lesions. Additional information obtained from the LUM data corroborated the remineralization kinetics affecting the PTR signals. The results pointed to enhanced effectiveness of subsurface lesion remineralization in the presence of fluoride.