Nanofertilizers comprising engineered nanoparticles (ENPs) have great potential in sustainable agriculture due to their strong capabilities of improving crop yields. As an effective fertilization strategy, foliar spraying could lead to broken and splashed ENP droplets, resulting in inaccurate leaf targeting and potential environmental contamination. Herein, we propose embedding Fe-based ENPs into a supramolecular hydrogel to effectively enhance the deposition amount on leaves and thus the bioavailability. The proper rheological properties of the hydrogel droplets and their robust interaction with soybean leaf simultaneously reduce the droplet rebound and fragmentation, especially under elevated impact speeds, resulting in up to 168.9% more droplet deposition compared to the ENP suspension. Computational fluid dynamics simulation analysis suggests that the contact angle is a key sensitive factor influencing the dynamic deposition behavior of the hydrogel droplet. A 15% reduction in the contact angle results in a 14% reduction of the highest bouncing height. The incorporation of ENPs enhances the viscous dissipation rate by 7.4% in comparison with pure hydrogel droplets. The hydrogel embedding also causes a 1.5-fold increase in ENP uptake compared to that of the ENP suspension. The hydrogel embedding delivers a reduction of 80% in the ENP application amount, compared to ENP suspensions, while achieving a 28% increase in the fresh weight of soybean seedlings. This work provides an effective method to enhance the deposition of ENPs during foliar application.