When plants are exposed to airborne particles, they can accumulate metals in their edible portions through root or foliar transfer. There is a lack of knowledge on the influence of plant exposure conditions on human bioaccessibility of metals, which is of particular concern with the increase in urban gardening activities. Lettuce, radish, and parsley were exposed to metal-rich ultrafine particles from a recycling factory via field atmospheric fallouts or polluted soil. Total lead (Pb) and cadmium (Cd) concentrations in of the edible plant parts and their human bioaccessibility were measured, and Pb translocation through the plants was studied using Pb isotopic analysis. The Pb and Cd bioaccessibility measured for consumed parts of the different polluted plants was significantly higher for root exposure (70% for Pb and 89% for Cd in lettuce) in comparison to foliar exposure (40% for Pb and 69% for Cd in lettuce). The difference in metal bioaccessibility could be linked to the metal compartmentalization and speciation changes in relation to exposure conditions. Metal nature strongly influences the measured bioaccessibility: Cd presents higher bioaccessibility in comparison to Pb. In the case of foliar exposure, a significant translocation of Pb from leaves toward the roots was observed. To conclude, the type of pollutant and the method of exposure significantly influences the phytoavailability and human bioaccessibility of metals, especially in relation to the contrasting phenomena involved in the rhizosphere and phyllosphere. The conditions of plant exposure must therefore be taken into account for environmental and health risk assessment.