In this work, the molecular interaction of the amino acid glycine and the mineral pyrite was performed to gain insight into the potential role of the mineral as a precursor of chemical complexity in the presence of ultraviolet (UV) radiation. Glycine samples were self-assembled on pyrite with and without exposure to UV radiation and subsequently characterized by scanning electron microscopy, infrared spectroscopy (with the second-derivative method), and AM1 and PM3 semi-empirical molecular computational simulations. In this work, our molecular modelling results suggest that pyrite acts as a template for self-assembly of glycine, and it is a potential catalyst for the glycine dimerization of relevance in interstellar space and ancient Earth conditions. A change in the structural complexity of glycine from the α to its γ polymorph when irradiated with UV radiation can be a condition for chemical evolution towards living forms.