Molecular vibrational spectroscopy is widely used in various sensing and imaging applications, providing intrinsic information at the molecular level. Nonlinear optical interactions using ultrashort laser pulses facilitate the selective coherent excitation of molecular vibrational modes by focusing energy into specific molecular bonds, boosting the signal level for multiple orders of magnitude. The dephasing of such coherence, which is susceptible to the local molecular environment, however, is often neglected. The unique capability of vibrational dephasing dynamics to serve as a unique probe for complex molecular interactions and the effect of local nano- and microenvironments are beyond the reach of conventional, intensity-based spectroscopy. Here, we developed a novel multiorder coherent Raman spectroscopy platform with a special focus on the temporal evolution of molecular vibrational dephasing, termed as time-resolved coherent Raman scattering (T-CRS) spectroscopy. By utilizing a high dynamic range detection, molecular vibrational dynamics and the environmental effects are demonstrated with multidimensional spectroscopic sensing, which promises a new range of applications in biology, materials, and chemical sciences.