Nickel slags can be produced through ferronickel preparation by the pyrometallurgical processing of laterite nickel ores; however, such techniques are underutilized at present, and serious environmental problems arise from the stockpiling of such nickel ores. In this study, a modification to the process of ferronickel preparation by the direct reduction of carbon bases in laterite nickel ores is proposed. The gangue from the ore is used as a raw material to prepare a cementitious material, with the main components of tricalcium silicate and tricalcium aluminate. By using FactSage software, thermodynamic calculations are performed to analyze the reduction of nickel and iron and the effect of reduction on the formation of tricalcium silicate and tricalcium aluminate. The feasibility of a coupled process to prepare ferronickel and cementitious materials by the direct reduction of laterite nickel ore and gangue calcination, respectively, is discussed under varying thermodynamic conditions. Different warming strategies are applied to experimentally verify the coupled reactions. The coupled preparation of ferronickel and cementitious materials with calcium silicate and calcium aluminate as the main phases in the same experimental process is realized.