Untangling the complex effects that different air pollution and climate change factors cause to forest ecosystems is challenging. Supersites, that is, comprehensive measurement sites where research and monitoring of the whole soil–plant–atmosphere system can be carried out, are suggested as a refinement of the current monitoring and research efforts in Europe. This chapter identifies and discusses key measurements to be carried out at such supersites, with a focus on four topical subjects: the carbon, nitrogen, ozone and water budgets. This kind of holistic approach is vital to a realistic translation of the ongoing changes in climate and air quality into research on the impacts on forest ecosystems. Such an integrated effort requires a considerable use of resources at highly instrumented measurement sites and can only be achieved by building on existing infrastructures.