Visible and ultraviolet upconversion (UC) emission is observed under 800 nm femtosecond laser excitation in LiNbO3 crystals triply doped with Tm3+, Yb3+, and Nd3+ at room temperature. Energy transfer (ET) from Nd3+ to Yb3+ then to Tm3+ is very important in this UC emission process. The overlapping between the emissions of D12→F34 and G14→H36, which makes up of blue emission band, is confirmed by transient investigation. From the pump energy dependence investigation, it is known that the dominant populating mechanism for the G14 state is the two-photon process, and that for D12 is the three-photon process. In our UC emission model, the G14 state is populated by the ET of F25/2(Yb3+)+H34(Tm3+)→F27/2(Yb3+)+G14(Tm3+), D12 state is populated by the ET of F32+H34→D12+H36 among Tm3+ ions. For LiNbO3 crystals doped with Tm3+ to the concentration of 0.9 mol %, the measured lifetimes of G14 and D12 are ∼80 and 4 μs.