Inspired by the mineralization process of bone, we have investigated mineralization on piezoelectric samples immersed in a solution with mineral ions. We have utilized polyvinylidene fluoride as a piezoelectric material and 10× simulated body fluid as a mineral solution. Three synthetic material systems were developed and characterized using scanning electron microscopy, X-ray diffraction, nanoindentation, and scratch testing. With these techniques, we provide insights into how the characteristics of the mineralization protocol affect the microstructure, chemical composition, crystal structure, and mechanical properties of the minerals. Increasing the solution temperature from 25 to 50 °C resulted in a greater packing density, roughly 10 times the stiffness and 4 times the fracture toughness. Collagen surface treatment resulted in roughly 7 times the stiffness along with potential anisotropy in the fracture toughness. Lastly, calcium phosphate minerals appear to pack in low-density and high-density phases on the piezoelectric scaffolds.