Biomineralization is a complex process in which the solution conditions, organic template, and crystal confinement coordinate to yield nanostructured composite materials with controlled optical and structural properties. Over the past few decades, research has examined various aspects of this mineralization process both by characterizing those found in nature and by creating synthetic composites. In particular, extensive research has been performed on CaCO3 crystallization growth and morphological control since CaCO3 is the most common inorganic component of biominerals. Recent work has shown that large single CaCO3 crystals with regularly spaced pores can be grown by stabilizing an amorphous calcium carbonate (ACC) intermediate through confinement and surface stabilization before the nucleation occurs. Our work extends this idea to show that arrays of anisotropic crystals can be grown with tunable sizes in the micrometer range through confinement on a micro-patterned surface and under a hydroscopic polymer film. These crystals appear to be uniaxially oriented with respect to the surface, and the resulting crystal morphology and orientation can be modified through the use of soluble growth modifiers. The resulting crystal morphology and sizes have been characterized by confocal light microscopy with cross-polarized filters and SEM.