The immense achievements of inelastic neutron scattering (INS) in recent years on the way to understanding the mechanism of high-temperature superconductivity were to a great extent enabled by the progress in fabricating large single-crystalline samples or coaligned mosaics consisting of up to several hundreds of individual single crystals. With the recent discovery of unconventional superconductivity in iron-based compounds, many of which can only be synthesized as relatively small crystals that rapidly decompose or deteriorate in air, we were faced with the technical challenge of preparing coaligned single-crystal arrays without exposing the samples to the ambient atmosphere. Here we describe a possible solution to this problem, which we have successfully employed to coalign both iron-pnictide and iron-chalcogenide single crystals in an argon atmosphere using a real-time digital x-ray Laue backscattering camera.