With a significantly increasing demand for miniaturized titanium thin-walled products, micro forming using sheet metals is a promising approach with high productivity. However, once the sheet thickness is scaled down to a micro-scale, there are many unknowns in terms of size effect and its affected fracture behavior. In this research, the influence of grain size on the fracture behavior of commercially pure titanium sheets with a thickness of 0.1 mm was investigated by the uniaxial tensile tests combined with a digital image correlation measurement system. The ductile-to-brittle transformation of fracture behavior with the grain size increasing from 33.07 to 107.70 μm was revealed. Macroscopically, the elongation and critical fracture stress of CP-Ti samples decrease with the increase of grain size. According to the scanning electron microscopic observations, the number of dimples decreases with grain size increasing, while the cleavage planes and river patterns gradually dominate in the coarse grain fracture surface. To explore the fracture mechanism, the dislocation evolution of various grain sizes is further observed by a transmission electron microscope. The dislocation emission from crack-tips was revealed at different grain sizes. Significant dislocation pile-up at grain boundaries was observed in the specimen with a grain size of 33.07 μm. Those intense dislocations reduce the effective stress at the crack tip resulting in higher crack propagation resistance. Nevertheless, the dislocation density at crack-tip decreases strongly with the increase of grain size leading to high crack-tip effective stress and less crack plasticity. Hence cleavage fracture was dominated in coarse grain CP-Ti sheets.