Temperature stable high-K LTCC material was prepared. The influence of fabrication process on the crystalline phases, microstructures and microwave dielectric properties of TiO2-Bi2O3-CuO ceramics were investigated. The crystalline phases and microstructures of TiO2-Bi2O3-CuO ceramics were investigated by X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy. It was found that rutile TiO2 phase and Bi2Ti4O11 phase co-existed in the TiO2-Bi2O3-CuO ceramics. Separate TiO2 grains and Bi2Ti4O11 grains distributed uniformly in the ceramic matrix. The composition 0.92TiO2-0.08Bi2Ti4O11 with 2 wt% CuO addition that was sintered at 900 °C for 2 h showed high dielectric constant (εr ~ 81), high quality factor (Q × f ~ 3,500 GHz) and near zero temperature coefficient of resonant frequency (τf ~ −5.1 ppm/°C), meanwhile the compatibility test showed that it could co-fire with silver electrode. The processing-microstructure-property interrelationship was also studied.