Nano zero-valent iron (nZVI) technologies have gained recognition for the remediation of heavily contaminated sites and reused as backfilling soil. The moisture environment at these sites not only impacts the reactions and reactivity of nZVI but also the dynamic responses of compacted backfilled soils. The research explored the effects of different nZVI dosages (0.2%, 0.5%, 1%, 2%, and 5%) on Lead-Zinc-Nickel ions contaminated soil under a controlled-moisture condition. Cyclic triaxial tests were performed to evaluate the dynamic responses of treated soil samples prepared using a consistent moisture compaction method. Particle size distribution and Atterberg limits tests assessed changes in particle size and plasticity. The study revealed a minor reduction in the particle size, liquid limit, plastic limit, and plasticity index of the contaminated soil. Notably, increasing nZVI dosages in treated soils led to growing Atterberg limits. An increase in the specific sand fraction of treated soils was observed with nZVI, suggesting nanoparticles–soil aggregations favoring existing larger particles. Stepwise loading cyclic triaxial tests indicated an optimal dynamic response of soil treated with 1% nZVI under the controlled-moisture condition, proven by notable enhancements in the maximum shear modulus, maximum shear stress, less shear strain, and higher damping ratio within the small strain range. It should be noted that moisture content in treated soils declined significantly with higher nZVI dosages during preparation, potentially impeding effective aggregation and the formation of a solid soil skeleton. These findings advance the importance of considering the balanced nZVI dosage and moisture content when employing the safety assessment of practical applications in both nano-remediation techniques and soil mechanics.