The further development of new processes utilizing liquid or supercritical CO2 as a solvent will benefit from the rational design of new CO2-philes. Understanding solvation structures and mechanisms of these molecules is an important part of this process. In such studies, determining the change in density as a function of the measured thermodynamic conditions (pressure and temperature) provides an excellent means of directly monitoring the solution conditions in the detection volume for a given technique. By integrating spectroscopic peaks, changes in area can be used to determine changes in analyte concentration in the detection volume, and thus, it should be possible to monitor the system density in situ. In the present study, we examine the utility of Raman and NMR spectroscopy as a means of following changes in solution density conditions and validate this approach in pure fluids and gases (N2 and CO2) and supercritical fluid mixtures (acetaldehyde vapor in N2). In addition, we present the design of a simple, inexpensive cell for conducting Raman and NMR measurements under moderate pressure conditions.