A new method for early caries diagnosis was proposed and tested through a home-made optical examination system that used quantitative light fluorescence (QLF) and digital imaging fiber optic transillumination (FOTI) (DIFOTI), with light sources across a wide spectral range, from 350 nm to 1,000 nm. The front-illuminated infrared light scattering image (FIR) showed similar diagnostic abilities to that of DIFOTI. The FIR method was invented based on the observation that caries lesions lose the high transmittance and low scattering properties of benign enamel tissue. There are various methods for the early diagnosis of caries, such as visual examination, exploration, X-ray radiography, QLF, FOTI, and infrared fluorescence (diagnodent). Among them, methods based on optical properties are regarded as having the most potential. A comparative study was performed between the FOTI, QLF, diagnodent, optical coherence tomography, and FIR scattering image methods, using 20 extracted teeth samples with early caries. A scale of lesion measurement based on optical image contrast was proposed. The statistical analysis showed a significant correlation between the DIFOTI and FIR methods (r = 0.35, p < 0.05). However, the QLF and diagnodent methods showed little association with FIR images, as they have different detection principles as compared with FIR. Tomographic images obtained by OCT, using 1,330 nm super luminescent LED as a gold standard of tooth structure, verified that the FOTI and FIR results correctly represented the lack of homogeneity in dental tissue. The newly proposed FIR method attained similar diagnostic results to those of FOTI, but with an easier approach.