We report the development of a microRNA (miRNA)-based theragnostic system that can facilitate simple therapeutic miRNA-34a delivery and visualization by high-resolution magnetic resonance (MR) imaging. Magnetic nanovectors were formed by directly attaching miRNA-34a to the surface of magnetic nanoparticles (MNPs), modified nitrosonium tetrafluoroborate (NOBF4) and subsequently introduced polyethylene glycol (PEG) molecules for high stability in an aqueous phase. The miRNA-34a?conjugated magnetic nanovectors showed therapeutic effects, inhibiting cellular migration and invasion through CD44 gene suppression; they also exhibited a strong MR signal. These results demonstrate that magnetic nanovectors have potential as theragnostic nanosystems for miRNA-based cancer therapy.