Er3+/Yb3+ co-doped TiO2 nanocrystals were prepared by Sol-gel method in which titanium tetrachloride was adopted as the precursor. The structure, particle size, and optical properties of samples were characterized by X-ray diffraction(XRD), Field emission-Scanning Electron Microscopy(FE-SEM) and photoluminescence(PL) spectra. Er3+ concentration was fixed at 1.0mol%, and Yb3+ concentration was changed from 3 to 10mol%. Intense upconversion luminescence was observed when the samples were excited by 980nm laser. The dependence of upconversion luminescence on Yb3+ concentration was presented. The results show that the upconversion luminescence increases with the Yb3+ concentration and gets its peak at 5%. The ratio of red emission to green emission(R/G) was strikingly enhanced with the increase of Yb3+ concentration. Under the excitation of 980nm, the green emission in the range of 520-570nm (2H11/2, 4S3/2→4I15/2) and the red emission in the range of 640~690nm (4F9/2 →4I15/2) are both due to two photons process. The possible upconversion mechanism was discussed.