The application of antiplant virus agents on leaf surfaces faces challenges due to their vulnerability to wear, instability, and limited duration, which in turn jeopardizes plant health and yield. In recent years, high-aspect-ratio nanomaterials have gained prominence as powerful carriers for disease treatment, thanks to their exceptional penetrability and precise drug delivery capabilities. Here, we synthesized a pH-responsive nanoimmune inducer (CNC-AMO) with strong leaf adhesion through a Schiff base reaction, achieved by grafting amino-oligosaccharides (AMOs) on the surface of aldehyde-based CNC (CNC−CHO). Fourier transform infrared spectrometry, zeta potential, X-ray photoelectron spectroscopy, X-ray diffraction, transmission electron microscopy, atomic force microscopy, scanning electron microscopy, thermogravimetric analysis, and elemental analysis were used to characterize the CNC-AMO. The CNC-AMO displayed the capability for pH-responsive AMO release, showcasing its potential for targeted and controlled delivery. When applied to plants, the CNC-AMO exhibited impressive anti-TMV efficacy during a weeklong observation period. Meanwhile, the CNC-AMO exhibited remarkable adhesion and scouring resistance on the surfaces of the plant leaves. We strongly believe that the synergy of environmentally friendly synthetic materials, efficient plant virus control, and streamlined scalability positions CNC-AMOs as a promising pesticide for plant virus therapy.