It is a great challenge to high colossal permittivity (CP, Ɛ r) in polycrystal ceramics together with low dielectric loss (tanδ) and high insulation resistivity (ρ) due to the miniaturization of electrical devices. In this contribution, the defect dipoles [ T i 4 + • e − C e S r • • − e • T i 4 + ] and [ C e S r • − e • T i 4 + ] have been actively induced in the Sr 1-1.5 x Ce x TiO 3 (SCT) systems by doping Ce ions with amphoteric nature to address this issue. The ultra-stable dielectric performance under the external stimulus, with Ɛ r = 12,406 (with low variation of < ±10%) and tanδ <0.08 , can be achieve in the x = 0.01 sample within the temperature range of 10–200 °C and at the frequencies ranging from 20 Hz to 1 MHz, accompanied by high insulation with ρ > 1010 Ω•cm with low degradation rate under harsh test conditions of 2–4.5 kV/cm. This work paves a path by multisite defect engineering to achieve high-performance CP ceramics. [ABSTRACT FROM AUTHOR]