Atmospherically deposited cadmium (Cd) may accumulate in plants through foliar uptake; however, the foliar uptake, accumulation, and distribution processes of Cd are still under discussion. Atmospherically deposited Cd was simulated using cadmium sulfide (CdS) with various particle sizes and solubility. Water spinach (Ipomoea aquatica Forsk, WS) and pak choi (Brassica chinensis L., PC) leaves were treated with suspensions of CdS nanoparticles (CdSN), which entered the leaves via the stomata. Cd concentrations of WS and PC leaves treated with 125 mg L−1 CdSN reached up to 39.8 and 11.0 mg kg−1, respectively, which are higher than the critical leaf concentration for toxicity. Slight changes were observed in fresh biomass, photosynthetic parameters, lipid peroxidation, and mineral nutrient uptake. Exposure concentration, rather than particle size or solubility, regulated the foliar uptake and accumulation of Cd. Subcellular and the high-resolution secondary ion mass spectrometry (NanoSIMS) results revealed that Cd was majorly stored in the soluble fraction and cell walls, which is an important Cd detoxification mechanism in leaves. The potential health risks associated with consuming CdS-containing vegetables were highlighted. These findings facilitate a better understanding of the fate of atmospheric Cd in plants, which is critical in ensuring food security.