Because of the small thermal capacity of ultrathin (similar to 200 nanometers) metal single crystals, it is possible to explore the coupling of catalytic and thermal action at low pressures. We analyzed a chemothermomechanical instability in this regime, in which catalytic reaction kinetics interact with heat transfer and mechanical buckling to create oscillations. These interacting components are separated and explored through experimentation, mathematical modeling, and scientific computation, and an explanation of the phenomenon emerges from their synthesis.