Terarylene frameworks containing benzothiazole as a photoprecursor of hydride donors are presented. We here report on two new scaffolds along with their photoreactivity in solution. Through use of selected external oxidants, the photogeneration of hydride donors is monitored using UV-visible, NMR, and TEM methods. As a proof-of-concept, photogeneration of hydride in the presence of Ag+ gave rise to the formation of Ag nanoparticles.