Due to their special properties, people have been increasingly interested in studying applications of nanoscale metal materials in environmental engineering. Literature about the current research on the synthesis, properties, and environmental applications of nanoscale iron-based materials is reviewed and summarized in this article. Different physical and chemical methods used for synthesizing nano-iron-based particles with desired size, structure, and surface properties are described. We also emphasize important properties of nano-iron-based particles, including the density and intrinsic reactivity of surface sites. These properties directly influence the chemical behavior of such particles and, consequently, affect their applications in water and wastewater treatment and in air pollution control. Environmental applications of nano-iron particles are discussed in detail, including removal of chlorinated organics, heavy metals, and inorganics.