Dielectric tunable composite ceramics Ba0.6Sr0.4 TiO3-Mg2TiO4 (BST-MT) are prepared with a heterogeneous nucleation sol-gel approach. The Mg2TiO4 powders are synthesized by the conventional solid-state reaction method. The micro-sized MT powders with dispersant Ciba-4010 are introduced into Ba-Sr-Ti sol to obtain uniform and homogeneous mixture compounds with nano-sized BST particles synthesized via heterogeneous nucleation (HN) in the sol-gel process. Thus, the microstructural and dielectric properties can be tailored. The dielectric constants of BST-MT composite ceramics can be adjusted in a large range from 294 to 1790, and the dielectric tunability can be adjusted from 29.4% to 37.0% with different MT contents from 60 wt% to 20 wt%. Compared to the samples prepared by the conventional solid-state (SS) process, the BST-MT composite ceramics by the heterogeneous nucleation sol-gel process exhibit a more uniform microstructure, and improve dielectric properties.