Synthesis of compositionally graded versions of PbZr1-xTixO3 thin films results in unprecedented strains ( as large as approximate to 4.5 x 10(5) m(-1)) and correspondingly unexpected crystal structures, ferroelectric domain structures, and properties. This includes the observation of built-in electric fields in films as large as 200 kV/cm. Compositional and strain gradients could represent a new direction of strain-control of materials.