Pure titanium composed of α single-phase has important applications for its excellent mechanical, physical, and chemical properties, which also impose high requirements on its surface finish. However, pure titanium is a difficult-to-machine material due to its low mass transportation caused by the low stiffness and the low thermal conductivity. Thus, it is greatly needed to investigate the machinability of pure titanium by precision grinding. In the present work, we carry out experimental and finite element simulation studies on the precision multi-grain grinding of pure titanium. Specifically, finite element model of pure titanium grinding using grinding wheel with multiple grains is established, which enables the prediction of successive material removal behavior by neighboring grains in line with experiments. The machining behavior of pure titanium and its correlation with machined surface morphology and grinding force are studied by experiment, and are further revealed by finite element simulation. Subsequent grinding experiments are performed to study the effects of workpiece speed and grinding depth on the ground surface quality of pure titanium, with which a surface roughness of 0.27 μm is obtained under the optimized grinding parameters.