Paleo-terrestrial sedimentary rare earth ore is a new type of rare earth ore, the process produces a large amount of rare earth residue after acid leaching separation of rare earth elements. Al, Fe, and Ti present in the rare earth residue are important metals, and the separation and extraction of metal elements from the rare earth residue can improve the utilization value of rare earth ores and solve the solid waste disposal problems. Sulfuric acid solution was used to leach the residue from rare earth ore processing to investigate the effect and reaction mechanism of sulfuric acid solution on the leaching behavior of Al, Fe, and Ti. The results showed that the sulfuric acid solution could effectively dissolve silica-aluminate and hematite in the rare earth ores, selectively leach Al and Fe. In contrast, anatase did not easily react with the sulfuric acid solution, and the leaching rate of Ti was low, which stayed in the leaching residue together with Si. The optimal reaction conditions were optimized using one-way and orthogonal experiments, and the leaching rates of Al, Fe and Ti reached 86.44%, 94.00%, and 7.14%, respectively, under the optimal reaction conditions of reaction temperature of 115℃, reaction time of 6 h, acid residue mass ratio of 2.1 g/g and liquid-solid ratio of 4 g/g. It was found that the reaction temperature significantly affected the leaching rates of Al and Fe. Then (NH4)2SO4 was added to the leaching solution, and Al could be converted to NH4Al(SO4)2 crystals and precipitated, and Al2O3 was produced by roasting to realize the separation of Al and Fe. This study realized the selective recovery of Al and Fe elements in rare earth residue, and enriched Si and Ti elements in the leaching residue, which was conducive to the recovery of Ti elements in the next step.