We describe the motivation, design, and execution of the Greenhouse gAs Uk and Global Emissions (GAUGE) project. The overarching scientific objective of GAUGE was to use atmospheric data to estimate the magnitude, distribution, and uncertainty of the UK greenhouse gas (GHG, defined here as CO2, CH4, and N2O) budget, 2013–2015. To address this objective we established a multi-year and interlinked measurement and data analysis programme, building on an established tall tower GHG measurement network. The inter-calibrated measurement network comprises ground-based, airborne, ship-borne, balloon-borne, and space-borne GHG sensors. Our choice of measurement technologies and measurement locations reflects the heterogeneity of UK GHG sources that range from small point sources such as landfills to large, diffuse sources such as agriculture. Atmospheric mole fraction data collected at the tall towers and on the ships provide information on sub-continental fluxes, representing the backbone to the GAUGE network. Additional spatial and temporal details of GHG fluxes over East Anglia were inferred from data collected by a regional network. Data collected during aircraft flights were used to study the transport of GHGs on local and regional scales. We purposely integrated new sensor and platform technologies into the GAUGE network, allowing us to lay the foundations of a strengthened UK capability to verify national GHG emissions beyond the project lifetime. For example, current satellites provide sparse and seasonally uneven sampling over the UK mainly because of its geographical size and cloud cover. This situation will improve with new and future satellite instruments, e.g. measurements of CH4 from the TROPOMI instrument aboard Sentinel-5P. We use global, nested, and regional atmospheric transport models and inverse methods to infer geographically resolved CO2 and CH4 fluxes. This multi-model approach allows us to study model spread in a posteriori flux estimates. These models are used to determine the relative importance of different measurements to infer the UK GHG budget. Attributing observed GHG variations to specific sources is a major challenge. Within a UK-wide spatial context we used two approaches: 1) Δ¹⁴CO2 and other relevant isotopologues (e.g. δ¹³CCH4) from collected air samples to quantify the contribution from fossil fuel combustion and other sources; 2) geographical separation of individual sources, e.g. agriculture, using a high-density measurement network. Neither of these represents a definitive approach, but they will provide invaluable information about GHG source attribution when they are adopted as part of a more comprehensive, long-term national GHG measurement programme. We also conducted a number of case studies, including an instrumented landfill experiment that provided a test-bed for new technologies and flux estimation methods. We anticipate that results from the GAUGE project will help inform other countries on how to use atmospheric data to quantify their nationally determined contributions to the Paris Agreement.