BaTiO3-SrTiO3 (BST) thick films (~ 250-390 μm) with layered structures were fabricated by tape-casting and lamination process. Layered composites with various Ba/Sr ratios were obtained by lamination of BaTiO3 (BT) and SrTiO3 (ST) tapes in different spatial configurations (2-2). As-prepared BST ceramics showed much improved sinterability over the laminates of pure BT or pure ST tapes. Dielectric properties of materials were measured in the temperature range of 25 °C to 200 °C. The method of utilizing of layered structures offered flexibility to maximize the energy storage capability at specific operating conditions: (temperature and electric field) by tailoring the dielectric properties through varying the spatial configurations of BT and ST films.