Copper-zinc-alumina catalysts are the industrially-used formulation for methanol synthesis from carbon monoxide and carbon dioxide containing feedstock. Its high performance stems from synergies that develop between its components. This important catalytic system has been investigated with a myriad of approaches, however, no comprehensive agreement has emerged as to the fundamental source of its high activity. One potential source of the disagreements is the considerable variation in pressure used in studies to understand a process that is industrially performed at pressures above 20 bar. Here, by systematically studying the catalyst state during temperature-programmed reduction and under carbon dioxide hydrogenation with in situ and operando X-ray absorption spectroscopy over four orders of magnitude in pressure, we show how the state and evolution of the catalyst is defined by its environment. Especially below 1 bar, the structure of the catalyst shows a strong pressure dependence. As pressure gaps are a general problem in catalysis, these observations have wide-ranging ramifications.The improvement of heterogeneous catalysts is central to a sustainable development of energy conversion and the production of chemicals. Historically, such development relied heavily on trial-and-error based research. More recently, advances in characterization methods allowed the study of catalysts under pretreatment and catalytic conditions, thus in situ and operando. This has permitted the possibility to derive fundamental understanding of the state of the catalyst whilst it is actually working 1 . Ideally, a detailed comprehension of the reaction mechanisms of the desired catalytic reaction emerges. Many of these methods, such as electron microscopy and X-ray photoelectron spectroscopy, remain limited in their routine application to pressure regimes in the millibar range [2][3][4][5] ; others, however, such as X-ray absorption spectroscopy (XAS) and X-ray diffraction (XRD), suffer no