Abstract: Using hydrotalcite (LDHs) as the carrier and ferric nitrate nonahydrate as the iron source, an iron nanoparticle-supported heterogeneous catalyst (Fe/LDHs) was successfully prepared by the impregnation method. This catalyst was used in the hydrogen borrowing reaction between aniline and benzyl alcohol to efficiently synthesize N-benzyl aniline. Using a single variable control strategy, the effects of reaction time, temperature, catalyst dosage and solvent type on the template reaction yield were systematically studied. The optimized reaction conditions were determined as follows: Reaction temperature 110 ℃, 0.3 mmol aniline, 0.6 mmol benzyl alcohol, 4 mg Fe/LDHs catalyst, petroleum ether as solvent, and reaction time 24 h. Under these conditions, the yield of the target product N-benzyl aniline can reach up to 97.6%. Further catalyst recycling experiments and substrate expansion studies confirmed that Fe/LDHs not only has excellent reuse stability, but also exhibits good substrate adaptability and universality.