A finite element method (FEM)-based simulation approach to predict the tunability in composite materials was developed and tested with analytical data. These tests showed good prediction capabilities of the simulation for the test data. The simulation model was then used to predict the tunability of a network-structured composite, where the dielectric phase formed clusters in a paraelectric network. This was achieved by simulating a reciprocal core-shell unit cell of said network. The simulation showed a high tunability for this network model, exceeding the tunability of the analytically evaluated layered, columnar, and particulate model. The simulation results were experimentally verified with a Ba0.6Sr0.4TiO3/Mg3B2O6 (BST/MBO) composite, where core-shell granulates were made with a two-step granulation process. These structured samples showed higher tunability and dielectric loss than the unstructured samples made for comparison. Overall, the structured samples showed higher tunability to loss ratios, indicating their potential for use in tunable radio frequency applications, since they may combine high performance with little energy loss.