Multiple-layer Lamina Emergent Mechanisms (MLEMs) are mechanisms made from multiple sheets (lamina) of material with motion that emerges out of the fabrication plane. This study has shown that understanding how layers are used in existing products and in nature provides insight into how MLEMs can also use layers to achieve certain tasks. The multi-layered nature of MLEMs and the interactions between these layers are what enhance the capabilities of MLEMs and allow them to better meet design objectives. Layer separation is one objective for which MLEMs are well-suited. Layer separation can have a variety of applications and there are a number of different ways to design a MLEM to achieve this objective. Single-layer LEM and MLEM designs could greatly benefit from suitable actuation techniques; those that are consistent with the advantages of these mechanisms and could be incorporated into their design. This work presents shape memory alloys, piezoelectrics and dielectric elastomers as suitable ways of actuating LEMs and MLEMs. A number of novel MLEMs are presented throughout this thesis.