The capability of liquid crystal elastomer (LCE) to program its shape changes in a reversible and controlled manner offer a multifunctional material platform, and are appealing in various applications including soft robots, smart surfaces, and tissue engineering substrates. Molecular alignment of LCEs is the key to enable the reversible and complex shape transformations at the macro- and microscale level. In this talk, I will present how we take advantage of unique properties of LCs to prepare macroscopically-aligned LCE monoliths. The chemistry for the LCE synthesis along with various alignment strategies will be highlighted. Depending on the initial alignment conditions, these reconfigurable soft materials can show a reversible switching between 2D sheets and complex 3D shapes when exposed to various external stimuli. The structure-property-actuation relationships of the LCEs will be further discussed.