We present a simple strategy to achieve excellent dielectric and nonlinear currentvoltage properties for pureCaCu3Ti4O12 ceramics prepared by a modified solgel method with different calcining conditions. At 1kHz and room temperature, the best CCTO ceramic can exhibit a high dielectric constant (e') of 9516 with a very low dielectric loss, tan d 0.020. The minimum value of tan d is 0.018 at 2.5kHz with e' 9433. High breakdown field of 4032V/cm and nonlinear coefficient of 7.05 were obtained.