Polyvinyl alcohol (PVA) is a hydrophilic polymer with various characteristics desired for biomedical applications and can be transformed into a solid hydrogel by physical crosslinking, using a low-temperature thermal cycling process. As with most polymeric materials, the mechanical properties of the resultant PVA are isotropic, as oppose to most soft tissues, which are anisotropic. The objective of this research is to develop a PVA-based hydrogel that not only mimics the nonlinear mechanical properties displayed by cardiovascular tissues, but also their anisotropic behavior. By applying a controlled strain to the PVA samples, while undergoing low-temperature thermal cycling, we were able to create oriented mechanical properties in PVA hydrogels. The oriented stress-strain properties of porcine aorta were matched simultaneously by a PVA hydrogel prepared (10% PVA, cycle 3, 75% initial strain). This novel technique allows the controlled introduction of anisotropy to PVA hydrogel, and gives a broad range of control of its mechanical properties, for specific medical device applications.