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This feature article summarizes recent advances in extrusion-based 3D printing of active materials in both non-living and living systems. 

Programmable 3D shape morphing of stimuli-responsive hydrogels is of great interest for the fabrication of soft actuators and robots. The corporation of hydrogel matrices and functional additives is discussed in this review. 

Tunable rheological responses are obtained by coupling temperature-responsive capillary networks with jammed microgels, which facilitate complex structures and scale-ups by 3D printing. 

Abstract Achieving a simple yet sustainable printing technique with minimal instruments and energy remains challenging. Here, a facile and sustainable 3D printing technique is developed by utilizing a reversible salting-out effect. The salting-out effect induced by aqueous salt solutions lowers the phase transition temperature of poly(N-isopropylacrylamide) (PNIPAM) solutions to below 10 °C. It enables the spontaneous and instant formation of physical crosslinks within PNIPAM chains at room temperature, thus allowing the PNIPAM solution to solidify upon contact with a salt solution. The PNIPAM solutions are extrudable through needles and can immediately solidify by salt ions, preserving printed structures, without rheological modifiers, chemical crosslinkers, and additional post-processing steps/equipment. The reversible physical crosslinking and de-crosslinking of the polymer through the salting-out effect demonstrate the recyclability of the polymeric ink. This printing approach extends to various PNIPAM-based composite solutions incorporating functional materials or other polymers, which offers great potential for developing water-soluble disposable electronic circuits, carriers for delivering small materials, and smart actuators. 

The stimuli-responsive self-folding structure is ubiquitous in nature, for instance, the mimosa folds its leaves in response to external touch or heat, and the Venus flytrap snaps shut to trap the insect inside. Thus, modeling self-folding structures has been of great interest to predict the final configuration and understand the folding mechanism. Here, we apply a simple yet effective method to predict the folding angle of the temperature-responsive nanocomposite hydrogel/elastomer bilayer structure manufactured by 3D printing, which facilitates the study of the effect of the inevitable variations in manufacturing and material properties on folding angles by comparing the simulation results with the experimentally measured folding angles. The defining feature of our method is to use thermal expansion to model the temperature-responsive nanocomposite hydrogel rather than the nonlinear field theory of diffusion model that was previously applied. The resulted difference between the simulation and experimentally measured folding angle ( i.e. , error) is around 5%. We anticipate that our method could provide insight into the design, control, and prediction of 3D printing of stimuli-responsive shape morphing ( i.e. , 4D printing) that have potential applications in soft actuators, robots, and biomedical devices.