Laser sinter technique for (Ta₂O₅)_1-x(TiO₂)_x (x is 0.3, 0.4 and 0.5, respectively) based ceramics was briefly introduced in this paper. Thermal compensation of (Ta₂O₅)_1-x(TiO₂)_x based negative temperature coefficient materials could be allowed by combination of laser sinter and annealing in oxygen, which tuned their dielectric temperature coefficient nearly to zero. Dielectric properties of specimens prepared by conventional sintering, laser sintering and its annealing sample in oxygen were analyzed by X-ray diffraction (XRD) and scanning electron microscope (SEM). The results showed that thermal compensation of the negative temperature coefficient materials related to the oxygen defect, and led to the change of their temperature coefficients.