Optical imaging technologies have revolutionized modern biomedical research. The invention of stimulated Raman scattering (SRS) microscopy provides a general vibrational imaging platform for biological systems. In the first part of this talk, I will present the development of electronic enhanced SRS micro-spectroscopy, which achieves sub-micromolar sensitivity under a tightly focused objective. By integrating ultrasensitive electronic pre-resonant SRS microscopy with the design of rainbow-like, bioorthogonal Raman dyes and an optimized tissue clearing strategy, we established a highly multiplexed volumetric imaging framework for spatial and molecular mapping of multiple proteins in intact brain tissues. The second part of the talk will highlight the development of ULTRA, an ultrarapid 3D histology pipeline. ULTRA is a label-free, stain-free, fixation-free, and section-free approach that enables rapid visualization of 3D histological architecture and tumor infiltration boundaries in gliomas. Fueled by the synergy between advanced spectroscopy and chemical innovation, Raman-based imaging technologies are gaining significant momentum and promise to drive new biological discoveries in the near future.