Provided herein are systems and methods for polymerizing and programming a liquid crystal polymer, including a liquid crystal elastomer (LCE) with two-way shape-memory via a stepped or self-limiting reaction. In the described method, the reaction may be stepped to achieve different aspects of the two-way shape-memory effect in the produced LCE. In one embodiment, the method creates a polydomain LCE body with a completed thiol-acrylate Michael addition reaction polymerization. The method may further crosslink the polydomain LCE body under a stimulus, thereby locking a domain state in a portion of the polymer. A two-way shape-memory effect of the LCE may thereafter be programmed and locked into the LCE the second stage polymerization reaction. The self-limiting reaction allows for unprecedented control over LCE domain states and cross-linking densities, as well as the resultant mechanical and optical properties of the LCE formed.