In most engineering applications, the coefficients of thermal expansion (CTEs) of different materials in integrated structures are inconsistent, especially for the thin-film multilayered coatings. Therefore, mismatched thermal deformation is induced due to temperature variation, which leads to an extreme temperature gradient, stress concentration, and damage accumulation. Controlling the CTEs of materials can effectively eliminate the thermally induced stress within the layered structures and thus considerably improve the mechanical reliability and service life. In this paper, randomly distributed fibers are incorporated into the matrix material and thus utilized to tune the material CTE from the macroscopical viewpoint. To this end, finite element (FE) modeling is proposed for fiber-reinforced matrix composites. In order to overcome the challenges of creating numerical models at a mesoscale, the random distribution of fibers in three-dimensional space is realized by proposing a fiber growth algorithm with the control of the in-plane and out-of-plane angles of fibers. The homogenization method is adopted to facilitate the FE simulations by using the representative volume element (RVE) of composite materials. Periodic boundary conditions (PBC) are applied to realize the prediction of the equivalent CTE of macroscopic composite materials with randomly distributed fibers. In the established FE model, the random distribution of carbon fibers in the matrix makes it possible to tune the CTE of the composite material by considering the orientation of fibers in the matrix. The FE predictions show that the volume fraction of carbon fibers in the composite materials is found to be crucial to macroscopic CTE, but results in minor variations in Young’s modulus and shear modulus. With the developed ABAQUS plug-in program, the proposed tuning method for CTE is promising to be standardized for industrial practice.