The structural regulations of Ba2LaF7 self-crystallized glass-ceramics were successfully analyzed by adjusting the concentration of the doped TiO2. Increasing the doping concentration of TiO2 tightened the internal structure of the glass and depleted the self-crystallization of Ba2LaF7. Further analysis revealed that TiO2 acts as a nucleating agent in the glass-ceramics. However, the number of the crystal nuclei increased, and the growth of the crystal grains was reduced. The change in the internal structure of the glass-ceramics was due to the varying self-crystallization process of Ba2LaF7 in the glass-ceramics and was not directly caused by the incorporation of TiO2.