The aim of this study was to investigate the effects of TiO₂/CaO addition on the crystallization and flexural strength of leucite glass-ceramics (GC). Synthesis of translucent and high strength GCs is important for the development of aesthetic and durable dental restorations. To achieve this, experimental aluminosilicate glasses (1–3 mol% TiO₂ and CaO (B1, B2, B3)) were melted in a furnace to produce glasses. Glasses were ball milled, screened and heat treated via crystallization heat treatments, and characterized using XRD, differential scanning calorimetry, dilatometry, SEM and biaxial flexural strength (BFS). Increasing nucleation hold time (1–3 h) led to a reduction in crystallite number for B2 and B3 GC, and significant differences in leucite crystal size at differing nucleation holds within and across test groups (p < 0.05). A high area fraction of leucite crystals (55.1–60.8%) was found in the GC, with no matrix microcracking. Changes in the crystal morphology were found with higher TiO₂/CaO addition. Mean BFS of the GC were 211.2–234.8 MPa, with significantly higher Weibull modulus (m = 18.9) for B3 GC. Novel glass compositions enriched with TiO₂/CaO led to crystallization of leucite GC of high aspect ratio, with high BFS and reliability. The study’s findings suggest a potential high performance translucent leucite GC for use in the construction of dental restorations.