Microwave dielectric ceramics with the composition of (1−x)Li 2 Zn 3 Ti 4 O 12 (LZT)–xTiO 2 (0≤x<1) were prepared by the solid-state reaction method. The crystal structures were determined by X-ray diffraction. (1−x)LZT–xTiO 2 solid solutions show a cubic structure [P4 3 32 (212)] similar to Zn 2 Ti 3 O 8 in the range of 0.2≤x≤0.4. When the x value reaches 0.6, the rutile TiO 2 phase appears. The microwave dielectric properties were studied by a Network Analyzer. The relative permittivity (ɛ r ) and temperature coefficients of resonant frequency (τ f ) were adjusted with increasing x values. Especially, 0.4LZT–0.6TiO 2 ceramic exhibits good microwave dielectric properties with a ɛ r of 25.1, a high Q×f of 62,000GHz and a near-zero τ f of −5.2ppm/°C.