Hydrogen bond (HB) networks are essential for stabilizing molecular structures in solution and govern the solubility and functionality of molecules in an aqueous environment. HBs are important in biological processes such as enzyme-substrate interactions, protein folding, and DNA replication. However, the exact role of weakly polarized C-H bonds as HB proton donors in solution, such as CH/ HBs, remains mostly unknown. Here, we employ a novel approach focusing on vibrational dephasing to investigate the coherence relaxation of induced dipoles in C-H bonds within CH/ HB networks, utilizing time-resolved coherent anti-Stokes Raman scattering (T-CARS) spectroscopy. Using a representative binary system of dimethyl sulfoxide (DMSO)-water, known for its C-H backboned HB system (, C-H���S), we observed an increase in the dephasing time of the C-H bending mode with increasing water content until a percolation threshold at a 6���:���1 water���:���DMSO molar ratio, where the trend is reversed. These results provide compelling evidence for the existence of C-H���S structures and underscore the presence of a percolation effect, suggesting a critical threshold where long-range connectivity is disputed.
