Diffuse Interstellar Bands (DIBs) are among the longest-standing mysteries in astronomy. These unidentified absorption features, observed throughout the interstellar medium, are believed to arise from complex carbon-rich molecules and hold crucial information about the cosmic carbon cycle, interstellar chemistry, and the conditions that precede star and planet formation. Our research aims to identify potential molecular carriers of DIBs by measuring the gas-phase spectroscopic fingerprints of large carbonaceous ions under astrophysically relevant conditions. Using a custom-built instrument that combines mass spectrometry, ion mobility spectrometry, and laser spectroscopy, we obtain spectra from the near-infrared to the ultraviolet range of mass- and shape-selected moleular ions for direct comparison with astronomical observations.