This review collects recent developments in the field of liquid crystalline elastomers (LCEs) with an emphasis on their use for actuator and sensor applications. Several synthetic pathways leading to crosslinked liquid crystalline polymers are discussed and how these materials can be oriented into liquid crystalline monodomains are described. By comparing the actuating properties of different systems, general structure–property relationships for LCEs are obtained. In the final section, how these materials can be turned into usable devices using different interdisciplinary techniques are described.