Data for "Large Area, High Resolution Mapping of Approximate Rotational Symmetries in a Pd77.5Cu6Si16.5 Metallic Glass Thin Film" by Shuoyuan Huang, Carter Francis, John Sunderland, Vrishank Jambur, Izabela Szlufarska, and Paul M Voyles. Contains molecular dynamics simulated structures of Al-Sm metallic glasses and electron nanodiffraction simulations from those structures, electron nanodiffraction data from Pd-Cu-Si metallic glass thin films under various experimental conditions, and analysis of those data using symmetry coefficients.