This joint theoretical and experimental study establishes that the adsorption of polycyclic aromatic hydrocarbons (PAHs) onto the amorphous ice surface provokes a broadening and redshift of the “dangling” OH (dOH) ice spectral feature, the redshift increasing with PAH size up to ∼85 cm^-1. It also reveals that, in certain interaction configurations, adsorption induces substantial reorganization of the hydrogen-bonding network at the ice surface. Comparison with experiments validates the novel theoretical methodology relying on the density functional-based tight binding approach, which offers a compromise between the system size and accuracy, enabling a wide sampling of surface structures. Applied in an astrophysical context, this study suggests that widening of the dOH feature by adsorption of aromatic molecules could explain its absence heretofore in observational ice spectra, offering hope that future missions with higher sensitivity will verify its presence or absence in dense regions.