Data sets used to prepare Figures 5, 7-11, 13 and S4-S7 in the Journal of Chemical Physics article entitled "Titanium phosphate glasses: Beyond tetrahedral network structures." The data sets describe the structure of glasses in the TiO2-P2O5 system as (i) measured using neutron and high-energy x-ray diffraction, Raman scattering and 31P solid-state nuclear magnetic resonance spectroscopy and (ii) simulated using ab initio molecular dynamics (AIMD). They also give the predictions of an analytical model for the glass structure and a comparison of these predictions with the results obtained from the diffraction and AIMD results.