© 2020 The Authors. Methods in Ecology and Evolution published by John Wiley & Sons Ltd on behalf of British Ecological Society In recent years, the availability of airborne imaging spectroscopy (hyperspectral) data has expanded dramatically. The high spatial and spectral resolution of these data uniquely enable spatially explicit ecological studies including species mapping, assessment of drought mortality and foliar trait distributions. However, we have barely begun to unlock the potential of these data to use direct mapping of vegetation characteristics to infer subsurface properties of the critical zone. To assess their utility for Earth systems research, imaging spectroscopy data acquisitions require integration with large, coincident ground-based datasets collected by experts in ecology and environmental and Earth science. Without coordinated, well-planned field campaigns, potential knowledge leveraged from advanced airborne data collections could be lost. Despite the growing importance of this field, documented methods to couple such a wide variety of disciplines remain sparse. We coordinated the first National Ecological Observatory Network Airborne Observation Platform (AOP) survey performed outside of their core sites, which took place in the Upper East River watershed, Colorado. Extensive planning for sample tracking and organization allowed field and flight teams to update the ground-based sampling strategy daily. This enabled collection of an extensive set of physical samples to support a wide range of ecological, microbiological, biogeochemical and hydrological studies. We present a framework for integrating airborne and field campaigns to obtain high-quality data for foliar trait prediction and document an archive of coincident physical samples collected to support a systems approach to ecological research in the critical zone. This detailed methodological account provides an example of how a multi-disciplinary and multi-institutional team can coordinate to maximize knowledge gained from an airborne survey, an approach that could be extended to other studies. The coordination of imaging spectroscopy surveys with appropriately timed and extensive field surveys, along with high-quality processing of these data, presents a unique opportunity to reveal new insights into the structure and dynamics of the critical zone. To our knowledge, this level of co-aligned sampling has never been undertaken in tandem with AOP surveys and subsequent studies utilizing this archive will shed considerable light on the breadth of applications for which imaging spectroscopy data can be leveraged.