Bauxite is the main source for alumina production. With the rapid development of iron and steel industry and aluminum industry, high-quality iron ore and bauxite resources become increasingly tense. However, a lot of iron-rich bauxite and Bayer red mud resources have not been timely and effectively recycled, resulting in serious problems of environmental pollution and wastage of resources. The comprehensive utilization of iron-rich bauxite and red mud is still a worldwide problem. The industrial stockpiling is not a fundamental way to solve the problems of ironrich bauxite and red mud. As to the recovery of valuable metals from iron-rich bauxite and red mud, there are a lot of technical and cost problems, which are serious impediments to industrial development. Applying red mud as construction materials like cement, soil ameliorant applications face the problem of Na, Cr, As leaching into the environment. However, the high-temperature reduction, smelting and alkaline leaching process is a feasible method to recover iron and alumina from iron-rich bauxite and red mud. This chapter intends to provide the reader an overview on comprehensive utilization technology of the low-grade iron-rich bauxite and Bayer red mud sources.