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Transparent bubble free phosphate glasses having a composition 40Na2O–10Al2O3–xTiO2–(50−x)P2O5 (x=0–20 mol%) were prepared by melt quench method and characterized for their optical, thermo‐physical and structural aspects. Substitution of TiO2 for P2O5 up to 10 mol% in the ternary 40Na2O–10Al2O3–50P2O5 glass increases the density, glass transition temperature (Tg), microhardness (MH), and decreases the molar volume, thermal expansion coefficient, and optical gap (Eoptical). Further substitution of TiO2 results in the decrease of density, Tg, and MH. Based on the 31P magic angle spinning nuclear magnetic resonance and Fourier transform infrared spectroscopy, it is established that up to 10 mol% TiO2 incorporation in the glass, the network undergoes only a slow depolymerization while forming P–O–Al and P–O–Ti linkages. Variation in optical properties like Eoptical and wavelength corresponding to emission maxima indicates that up to 10 mol% incorporation, TiO2 acts as a network modifier and above that it forms a network of Ti–O–Ti linkages connected with discrete PO4 structural units. Thus, the variation in the thermo‐physical and optical properties has been explained by the composition‐dependent structural changes brought about by TiO2 in the glass matrix.