Liquid crystalline materials (LCMs) showcase extensive potential for application in a range of industries including soft robotics, optics, and, more recently, biomaterials. By patterning the mesogen alignment within these materials, a directed response can be achieved resulting in muscle-like contraction or 3-D deformation. Employing alignment techniques such as surface enforced alignment, photopatterning, and 3-D printing, we seek to further develop these methods to target biologically relevant LCM applications. Here, I will discuss two LCM systems that highlight recent progress in liquid crystalline biomaterials as enzymatic biosensors and substrates for tissue engineering. In the development of the biosensors, we explore the implications of harnessing an enzyme (jack bean urease) within a heavily crosslinked liquid crystalline network (LCN). The network leverages a hydrogen-bonded liquid crystalline mesogen as a chemoresponsive unit, sensitizing the material to ammonia. As the urease enzyme catalyzes the transformation of urea into ammonia, the pre-programmed alignment of the network mesogens is disrupted, resulting in a bulk shape change. In a separate study, surface aligned liquid crystalline elastomers are synthesized to target aligned cell culture for anisotropic tissues such as muscle. Results show a preference for cell growth along the nematic director of LCEs.