The aim of this study was to analyse the predictive power of several clinical baseline parameters and the de-/remineralisation properties of in vivo etched sites measured with quantitative light-induced fluorescence (QLF) for subsequent 2-year caries increment. At baseline, in 44 children (8.23 ± 1.5 years) two areas (diameter 2 mm) of the buccal surface of a primary posterior tooth were etched with 36% phosphoric acid gel for 1 and 4 min, respectively. The etched sites were analysed immediately after etching (ΔQ1) and 24 h (ΔQ2) later by QLF. Additionally, caries status (deft/DMFT and initial caries), approximal plaque, bleeding on probing, and the patient’s current use of fluorides were recorded. In the 2-year follow-up, 29 children were re-assessed. After clinical examination, the caries increment was calculated (ΔDMFT) and correlated with the baseline clinical variables and the QLF readings. Results showed a significant positive correlation between ΔQ1 min and the ΔDMFT (r = 0.44, p = 0.02). The ΔDMFT was significantly correlated with the baseline deft (r = 0.56, p = 0.002), cavitated active caries lesions (r = 0.52, p = 0.003), and filled teeth (r = 0.53, p = 0.003). In a regression analysis the use of fluoridated salt (SC = –0.10) and fluoride gel (SC = –0.14) were negatively associated with ΔDMFT. In conclusion, these findings suggest that the demineralisation properties of the etched sites and the outcome of the 24-hour measurements with QLF are significantly associated with caries increment. Previous caries experience strongly correlated with caries increment in this group of children.