Three radiological dispersal devices were detonated in 2012 under controlled conditions at Defence Research and Development Canada's Experimental Proving Grounds in Suffield, Alberta. Each device comprised a 35-GBq source of La. The dataset obtained is used in this study to assess the MLCD, ADDAM, and RIMPUFF atmospheric dispersion models. As part one of a two-part study, this paper focuses on examining the capabilities of the above three models and evaluating how well their predictions of air concentration and ground deposition match observations from the full-scale RDD experiments.