The design and synthesis of soft polymeric materials with tailored properties is an area of emphasis in our group. This talk will focus on two unique materials, covering synthesis through properties, revealing structure property relationships as we now understand them. (i) The first part of the talk will examine new liquid crystalline elastomers that allow either one-way or two-way shape memory behavior, depending on underlying phase behavior dictated by chemical composition. Uses of these materials as reversible embossing media and artificial muscles will be discussed. (ii) Next, I will discuss hybrid hydrogels that combine the inorganic-organic POSS moiety (polyhedral oligomeric silsesquioxane) with hydrophilic groups in a multiblock architecture. The resulting thermoplastic hydrogels allow tuning of equilibrium swelling and mechanical properties, with unusual durability being observed in comparison to acrylamide-type hydrogels.