Atmospheric deposition plays a significant role in introducing cadmium (Cd) into agroecological systems; however, accurately determining its accumulation in crops through foliar and root uptake presents challenges. This study investigated the bioaccumulation of atmospherically deposited Cd in soybean using a three-year fully factorial atmospheric exposure experiment incorporating Cd isotope analysis. Results shown that atmospheric deposition accounted for 1−13% of soil Cd pools, yet contributed 11−72% of Cd to soybean tissues during the growing seasons. Over the course of soil exposure to atmospheric deposition ranging from 1 to 3 years, no notable variations were observed in Cd concentrations in soil solutions and soybean tissues, nor in isotope ratios. Newly deposited Cd was a major source in soybean plants, and the bioavailability of deposited Cd rapidly aged in soils. Atmospheric Cd enriched in lighter isotopes induced negative isotope shifts in soybean plants. By employing an optimized isotope mixing model in conjunction with a mass balance approach, foliar Cd uptake contributed 13− 51%, 16−45%, and 21−56% to stem, leaf, and seed, respectively. This study highlights substantial contribution of foliar uptake of atmospheric deposition to Cd levels in soybean and controlling foliar uptake as a potential strategy in agroecological systems experiencing high atmospheric Cd deposition.