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A novel large-pore titanosilicate with YFItopology, [Ti]-YNU-5, was prepared via post-synthetic isomorphous substitution of Ti for Al in the YFIframework. It exhibited the enhanced catalytic performances in the liquid-phase epoxidation of bulky alkenes and the oxidation of phenol with hydrogen peroxide. Hydrophobicity was found to be an important factor.Graphical AbstractThe preparation of large-pore YFI-type titanosilicate, [Ti]-YNU-5, via post-synthetic isomorphous substitution of Ti for Al is reported. Improved hydrophobicity by decreasing silanol groups makes it an effective catalyst for selective oxidations, especially cyclooctene epoxidation.