In recent years, nanoscale zero-valent iron (nZVI) has been gradually applied in soil remediation due to its strong reducing ability and large specific surface area. Compared to conventional remediation solutions, in situ remediation using nZVI offers some unique advantages. In this review, respective merits and demerits of each approach to nZVI synthesis are summarized in detail, particularly the most commonly used aqueous-phase reduction method featuring surface modification. In order to overcome undesired oxidation and agglomeration of fresh nZVI due to its high reactivity, modifications of nZVI have been developed such as doping with transition metals, stabilization using macromolecules or surfactants, and sulfidation. Mechanisms underlying efficient removal of organic pollutants enabled by the modified nZVI lie in alleviative oxidation and agglomeration of nZVI and enhanced electron utilization efficiency. In addition to chemical modification, other assisting methods for further improving nZVI mobility and reactivity, such as electrokinetics and microbial technologies, are evaluated. The effects of different remediation technologies and soil physicochemical properties on remediation performance of nZVI are also summarized. Overall, this review offers an up-to-date comprehensive understanding of nZVI-driven soil remediation from scientific and practical perspectives.