Mobile source emission models for years have depended on laboratory-based dynamometer data. Recently, however, portable emission measurement systems (PEMS) have become commercially available and in widespread use, and make on-road real-world measurements possible. As a result, the newest mobile source emission models (e.g., U.S. Environmental Protection Agency’s mobile vehicle emission simulator) are becoming increasingly dependent on PEMS data. Although on-road measurements are made under more realistic conditions than laboratory-based dynamometer test cycles, they introduce influencing variables that must be carefully measured for properly developed emission models. Further, test programs that simply measure in-use driving patterns of randomly selected vehicles will result in models that can effectively predict current-year emission inventories for typical driving conditions. However, when predicting more aggressive transportation operations than current typical operations (e.g., higher speeds, accelerations), the model predictions will be less certain. In this paper, various issues associated with on-road emission measurements and modeling are presented. Further, an example on-road emission data set and the reduction in estimation error through the addition of a short aggressive driving test to the in-use data are examined. On the basis of these results, recommendations are made on how to improve the on-road test programs for developing more robust emission models.