Vegetation can form a barrier between traffic emissions and adjacent areas, but the optimal configuration and plant composition of such green infrastructure (GI) are currently unclear. We examined the literature on aspects of GI that influence ambient air quality, with a particular focus on vegetation barriers in open-road environments. Findings were critically evaluated in order to identify principles for effective barrier design, and recommendations regarding plant selection were established with reference to relevant spatial scales. As an initial investigation into viable species for UK urban GI, we compiled data on 12 influential traits for 61 tree species, and created a supplementary plant selection framework. We found that if the scale of the intervention, the context and conditions of the site and the target air pollutant type are appreciated, the selection of plants that exhibit certain biophysical traits can enhance air pollution mitigation. For super-micrometre particles, advantageous leaf micromorphological traits include the presence of trichomes and ridges or grooves. Stomatal characteristics are more significant for sub-micrometre particle and gaseous pollutant uptake, although we found a comparative dearth of studies into such pollutants. Generally advantageous macromorphological traits include small leaf size and high leaf complexity, but optimal vegetation height, form and density depend on planting configuration with respect to the immediate physical environment. Biogenic volatile organic compound and pollen emissions can be minimised by appropriate species selection, although their significance varies with scale and context. While this review assembled evidence-based recommendations for practitioners, several important areas for future research were identified.