Raman spectroscopy is employed successfully for analysis of hydrogen isotopologues at the Tritium Laboratory Karlsruhe (TLK). In this paper, we summarize the recent achievements in the further development on this technique, and the various applications for which it is used at the TLK. Further, we show that Raman spectroscopy has evolved as a versatile, highly accurate key method for quantitative analysis complementing the portfolio of analytic techniques at the TLK.