SrTiO3/Zr2P2WO12 dielectric ceramic composites with controllable coefficient of thermal expansion (CTE) were prepared by using the solid-state method, and X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive spectrometry (EDS) spectrum were used to analyze its composition and microstructure. The coefficients of thermal expansion and dielectric properties were measured with a dilatometer and precision impedance analyzer, respectively. Results showed that the solid-state method was effective in obtaining composites with controllable thermal expansion coefficients (9.23–2.37) × 10−6/K and dielectric constants (17.15–39.56, 1 MHz) by combining the negative thermal expansion materials Zr2P2WO12 and SrTiO3.