A system for measuring the two-dimensional (2-D) spatial distribution of atmospheric CO2 over complex industrial sites and urban areas on the order of 1 to 30 km2 every few minutes with a spatial resolution as high as tens of meters has been developed and demonstrated over the past 3 years. The greenhouse gas (GHG) laser imaging tomography experiment (GreenLITE™) provides improved measurement capabilities for applications ranging from automated 24/7 monitoring of ground carbon storage/sequestration (GCS) sites to long-duration real-time analyses of GHG sources and sinks in urban environments. GreenLITE combines a set of sensors based on an intensity modulated continuous wave approach with 2-D sparse tomographic reconstruction mechanisms to compute a 2-D map of CO2 concentrations over the area of interest. GreenLITE systems have recently been deployed at a number of test facilities, including a 4000-h demonstration at a GCS site in Illinois and an urban deployment in Paris, France, from November 2015 to the present. This paper describes the GreenLITE concept and the associated measurement capabilities and provides proof of concept results and analyses of observations from both short-term tests as well as longer-term industrial and urban deployments.