The lunar surface evolves over time due to space weathering, and the visible–near-infrared spectra of more mature (i.e., heavily weathered) soils are lower in reflectance and steeper in spectral slope (i.e., darker and redder) than their immature counterparts. These spectral changes have traditionally been attributed to the space-weathered rims of soil grains (and particularly nanophase iron therein). However, understudied thus far is the spectral role of agglutinates—the agglomerates of mineral and lithic fragments, nanophase iron, and glass that are formed by micrometeoroid impacts and are ubiquitous in mature lunar soils. We separated agglutinates and non-agglutinates from six lunar soils of varying maturity and composition, primarily from the 125–250 μm size fraction, and measured their visible–near-infrared reflectance spectra. For each soil, agglutinate spectra are darker, are redder, and have weaker absorption bands than the corresponding non-agglutinate and unsorted soil spectra. Moreover, greater soil maturity corresponds to darker agglutinate spectra with weaker absorption bands. These findings suggest that agglutinates (rather than solely the space-weathered rims) play an important role in both the darkening and reddening of mature soils—at least for the size fractions examined here. Comparisons with analog soils suggest that high nanophase iron abundance in agglutinates is likely responsible for their low reflectance and spectrally red slope. Additional studies of agglutinates are needed, both to more comprehensively characterize their spectral properties (across size fractions and in mixing with non-agglutinates) and to assess the relative roles of agglutinates and rims in weathering-associated spectral changes.