Calcium copper titanate powders were synthesized by a soft chemistry route, aiming to establish a cost-effective solution method to obtain sintered ceramics with giant electric permittivity (ε′) and low dissipation factor (tanδ). Powders and sintered pellets were characterized by several techniques. The thermal decomposition behavior of the porous foam evidences that a hydroxycitrate was formed below 200 °C. Single cubic perovskite-type phase was obtained after calcination of the precursor powder at 700 °C for 5 h. Negligible mass loss occurs above 400 °C. During heating the precursor material, CuO is the first crystallized phase. A giant ε′ and low tanδ are obtained after sintering. The extension of the thermal window of ε′ is wider than those of powders prepared by other methods.