With mineral resources becoming gradually more deficient, as well as the issue of mine tailings causing environmental pollution, more and more people have realized the great significance of tailings utilization. Iron ore tailings, as a kind of secondary resource, have been developed in recycling industries. The feasibility to produce forsterite refractory from high-silicon iron tailings and high-magnesium raw materials were discussed. Also, the synthesis reaction processes were studied from the results of the laboratory experiments. The experiments showed that the synthesis processes can be separated into three steps when using iron tailings to synthesize forsterite: (1) produce magnesium iron sosoloid (Mg(1-X)Fe(X)O) and magnesium metasilicate (MgSiO3), (2) form the fayalite, and (3) create the forsterite. The synthetic productions are primarily forsterite, hortonolite, and small amounts of magnesium metasilicate (MgSiO3). The hortonolite is wrapped around the surface of the forsterite particles and formed the cementing phase. In addition, the method to produce forsterite refractory and lightweight forsterite refractory from iron tailings were offered.