ULF Raman spectroscopy utilizes novel VHG filters to spectrally clean up the laser line before ULF Raman spectroscopy is measured with a single grating spectrometer in conjunction with CCD camera. The availabilityaccessibility of UFL Raman spectroscopy opens new opportunity to reveal key information such as intermolecular structure characterization, pharmaceutical polymorph identification,material phaseinterfacial structure determination.