Thin films of inorganic materials are used in diverse applications, typically in polycrystalline form due to their relatively simple production. We have used enhanced piezoresponse force microscopy to investigate the domain distribution within neighbouring grains in thin polycrystalline films of the ferroelectric–ferroelastic system lead zirconate titanate (PZT). We demonstrate that domains are organized into areas with a correlated alignment of the ferroelastic and ferroelectric domains, spanning multiple grain boundaries. We present five typical arrangements of such structures: azimuthal, radial, gradient, and short- and long- range linear domain organizations. Moreover, we discuss the mechanical and electrical constraints that dictate these structures.