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Abstract Laboratory‐based mid‐infrared (MIR) spectroscopy of terrestrial and planetary analogue materials, combined with chemical and spectral insights from mission‐derived data, provides critical tools for advancing our knowledge of planetary surfaces. The returned lunar samples provide information on the chemical variability of the lunar surface. Lunar basalts are notably enriched in TiO 2 when compared to their terrestrial equivalents, and are ideal candidates to study the influence of composition on MIR spectral features. We characterized 25 synthetic lunar glasses with variable TiO 2 (0.6–18.7 wt%) and SiO 2 (35.6–52.1 wt%) in the thermal infrared range using micro‐Fourier Transform Infrared Spectrometry (μ‐FTIR). Our data reveal a strong linear relationship between the intensity of a spectral shoulder at 14.25 μm (702 cm −1 ) and the TiO 2 content of the analyzed glasses. We suggest that the relationship in our samples reflects an increased distortion of the silicate network with increasing TiO 2 concentrations. We observe that TiO 2 acts as a network former in specific concentration intervals, thereby affecting the intensity of the observed spectral features in the MIR. This linear relationship is virtually nonexistent in samples that are developing stages of short‐range order in the glasses and those samples that show only moderate to low amounts of TiO 2 . Comparison with data sets from Earth and Mercury analogue materials confirms that the Christiansen Feature (CF) consistently correlates with the SiO 2 content, underscoring its robustness as a proxy for glass polymerization across planetary compositions. Finally, we emphasize that incipient crystal nucleation in glassy surfaces affects spectral features in the MIR range.