In recent years, 3D printing techniques have provided new opportunities for the fast and custom fabrication of high-quality parts. New developments in 4D printing looks to create structures which change their shape over time. Through the design of new shape memory polymer composites (SMPCs) and the application of new printing methods and techniques, the current state of additive manufacturing technologies is being advanced. Herein, three primary studies are conducted:​ 1) a literature review on the potential of 4D printing custom, wearable devices for biomedical applications, 2) the material development and characterization of a new SMPC featuring 2D MXene flakes and the design of large-scale deformation 4D printed structures, and 3) the characterization of a new porous printing technique for the development of a hybrid 4D printed actuating/sensing wearable device. Through these studies, a holistic view of 3D printing is provided, including material development and manufacturing, with the intention of continued innovation in 4D printing.