Environmentally benign (1-x)Ba(Ti 0.8 Zr 0.2 )O 3 -x(Ba 0.7 Ca 0.3 )TiO 3 (BZT-BCT) ceramics are promising materials due to their remarkable high piezoresponse [Liu and Ren, Phys. Rev. Lett. 103, 257602 (2009)]. In this Letter, by focusing on local and average structure in combination with macroscopic electromechanical and dielectric measurements we demonstrate the structure property relationship in the tetragonal BZT-BCT ceramic. During high-temperature cubic to tetragonal phase transformation, polar nanoregions are manifested through the spontaneous volume ferroelectrostriction at temperatures below ∼477 K. Temperature-dependent local structural investigations across the Zr K edge extended x-ray absorption fine-structure spectroscopy reveal an anomalous collaboration between the ZrO 6 and TiO 6 octahedra. These octahedra compromise their individuality during polarization development. The presence of domains of submicron size embedded inside the macroscopic ferroelectric regions below T m , as well as their hierarchical arrangement, is observed by piezoresponse force microscopy. Effects of the existence of the structural/polar heterogeneities below T m are observed also when polarizabilities of the poled and unpoled samples are compared; the poled sample is found to be more susceptible to the electric field. In addition, by using electric field dependent x-ray diffraction studies we also show that this ceramic under field exhibits a reduction of tetragonal distortion, which is consistent with earlier reports.