In this paper we report the development of thin films composed of two piezoelectric materials, namely (Ba(Ti0.8Zr0.2)O3-x(Ba0.7Ca0.3)TiO3 (BCTZ) and polyvinylidene difluoride (PVDF), thus obtaining high piezoelectric hybrid heterostructures for making them a viable option for wearable pressure sensors. The piezoelectric output response as a function of different weight percentage of BCTZ ceramic powders (x = 0.50 BCTZ50 and x = 0.55 BCTZ55) in the PVDF matrix was investigated. The highest value of the piezoelectric coefficient d33 and the capacitance, with low dielectric loss was obtained for the heterostructure composed of PVDF/BCTZ50.