Thin LiTaO3 films were prepared by spin coating of polymerized sol-gel precursor solution. Films have been deposited on single crystal silicon substrate, Ti/Pt or SiO2 coated silicon substrate. Films were characterized by x-ray diffraction, dielectric and pyroelectric Measurements. High Curie temperature (above 550 °C) was assumed for LiTaO3 thin films from the temperature dependence of dielectric constant. Replacing 35% of tantalum by titanium atoms in the LiTaO3 precursor solution has resulted the thin films with Curie temperature of 330 °C. The lower Curie temperature leads to the larger pyroelectric coefficient at room-temperature, which is more than double that of the undoped LiTaO3 thin films. The dielectric, pyroelectric, and ferroelectric properties have been compared to the single crystal LiTaO3 and ceramic Li0.91Ta0.73Ti0.36O3. LiTaO3 thin films are available by sol-gel process at low temperature, and their properties may possibly be controlled by varying the composition of the sol-gel precursor solution.