RESOURCES

Abstract
Abstract Mechanical gradients are useful to reduce strain mismatches in heterogeneous materials and thus prevent premature failure of devices in a wide range of applications. While complex graded designs are a hallmark of biological materials, gradients in manmade materials are often limited to 1D profiles due to the lack of adequate fabrication tools. Here, a multimaterial 3D‐printing platform is developed to fabricate elastomer gradients spanning three orders of magnitude in elastic modulus and used to investigate the role of various bioinspired gradient designs on the local and global mechanical behavior of synthetic materials. The digital image correlation data and finite element modeling indicate that gradients can be effectively used to manipulate the stress state and thus circumvent the weakening effect of defect‐rich interfaces or program the failure behavior of heterogeneous materials. Implementing this concept in materials with bioinspired designs can potentially lead to defect‐tolerant structures and to materials whose tunable failure facilitates repair of biomedical implants, stretchable electronics, or soft robotics.

Abstract
Soft actuation allows robots to interact safely with humans, other machines, and their surroundings. Full exploitation of the potential of soft actuators has, however, been hindered by the lack of simple manufacturing routes to generate multimaterial parts with intricate shapes and architectures. Here, we report a 3D printing platform for the seamless digital fabrication of pneumatic silicone actuators exhibiting programmable bioinspired architectures and motions. The actuators comprise an elastomeric body whose surface is decorated with reinforcing stripes at a well-defined lead angle. Similar to the fibrous architectures found in muscular hydrostats, the lead angle can be altered to achieve elongation, contraction, or twisting motions. Using a quantitative model based on lamination theory, we establish design principles for the digital fabrication of silicone-based soft actuators whose functional response is programmed within the material's properties and architecture. Exploring such programmability enables 3D printing of a broad range of soft morphing structures.

Abstract
Abstract Self-healing silicones that are able to restore the functionalities and extend the lifetime of soft devices hold great potential in many applications. However, currently available silicones need to be triggered to self-heal or suffer from creep-induced irreversible deformation during use. Here, we design and print silicone objects that are programmed at the molecular and architecture levels to achieve self-healing at room temperature while simultaneously resisting creep. At the molecular scale, dioxaborolanes moieties are incorporated into silicones to synthesize self-healing vitrimers, whereas conventional covalent bonds are exploited to make creep-resistant elastomers. When combined into architectured printed parts at a coarser length scale, layered materials exhibit fast healing at room temperature without compromising the elastic recovery obtained from covalent polymer networks. A patient-specific vascular phantom is printed to demonstrate the potential of architectured silicones in creating damage-resilient functional devices using molecularly designed elastomer materials. This article is protected by copyright. All rights reserved

Abstract
The weak mechanical properties of hydrogels due to the inefficient dissipation of energy in the intrinsic structures limit their practical applications. Here, a double-network (DN) hydrogel has been developed by integrating an ionically cross-linked agar network, a covalently cross-linked acrylic acid (AAC) network, and the dynamic and reversible ionically cross-linked coordination between the AAC chains and Fe3+ ions. The proposed model reveals the mechanisms of the improved mechanical performances in the DN agar/AAC-Fe3+ hydrogel. The hydrogen-bond cross-linked double helices of agar and ionic-coordination interactions of AAC-Fe3+ can be temporarily sacrificed during large deformation to readily dissipate the energy, whereas the reversible AAC-Fe3+ interactions can be regenerated after stress relief, which greatly increases the material toughness. The developed DN hydrogel demonstrates a remarkable stretchability with a break strain up to 3174.3%, high strain sensitivity with the gauge factor being 0.83 under a strain of 1000%, and good 3D printability, making the material a desirable candidate for fabricating flexible strain sensors, electronic skin, and soft robots.
The weak mechanical properties of hydrogels due to the inefficient dissipation of energy in the intrinsic structures limit their practical applications. Here, a double-network (DN) hydrogel has been developed by integrating an ionically cross-linked agar network, a covalently cross-linked acrylic acid (AAC) network, and the dynamic and reversible ionically cross-linked coordination between the AAC chains and Fe3+ ions. The proposed model reveals the mechanisms of the improved mechanical performances in the DN agar/AAC-Fe3+ hydrogel. The hydrogen-bond cross-linked double helices of agar and ionic-coordination interactions of AAC-Fe3+ can be temporarily sacrificed during large deformation to readily dissipate the energy, whereas the reversible AAC-Fe3+ interactions can be regenerated after stress relief, which greatly increases the material toughness. The developed DN hydrogel demonstrates a remarkable stretchability with a break strain up to 3174.3%, high strain sensitivity with the gauge factor being 0.83 under a strain of 1000%, and good 3D printability, making the material a desirable candidate for fabricating flexible strain sensors, electronic skin, and soft robots.

Abstract
Abstract The integration of biological systems into robotic devices might provide them with capabilities acquired from natural systems and significantly boost their performance. These abilities include real-time bio-sensing, self-organization, adaptability, or self-healing. As many muscle-based bio-hybrid robots and bio-actuators arise in the literature, the question of whether these features can live up to their expectations becomes increasingly substantial. Herein, the force generation and adaptability of skeletal-muscle-based bio-actuators undergoing long-term training protocols are analyzed. The 3D-bioprinting technique is used to fabricate bio-actuators that are functional, responsive, and have highly aligned myotubes. The bio-actuators are 3D-bioprinted together with two artificial posts, allowing to use it as a force measuring platform. In addition, the force output evolution and dynamic gene expression of the bio-actuators are studied to evaluate their degree of adaptability according to training protocols of different frequencies and mechanical stiffness, finding that their force generation could be modulated to different requirements. These results shed some light into the fundamental mechanisms behind the adaptability of muscle-based bio-actuators and highlight the potential of using 3D bioprinting as a rapid and cost-effective tool for the fabrication of custom-designed soft bio-robots.

Abstract
Abstract Stimuli-responsive materials have the potential to enable the generation of new bioinspired devices with unique physicochemical properties and cell-instructive ability. Enhancing biocompatibility while simplifying the production methodologies, as well as enabling the creation of complex constructs, i.e., via 3D (bio)printing technologies, remains key challenge in the field. Here, a novel method is presented to biofabricate cellularized anisotropic hybrid hydrogel through a mild and biocompatible process driven by multiple external stimuli: magnetic field, temperature, and light. A low-intensity magnetic field is used to align mosaic iron oxide nanoparticles (IOPs) into filaments with tunable size within a gelatin methacryloyl matrix. Cells seeded on top or embedded within the hydrogel align to the same axes of the IOPs filaments. Furthermore, in 3D, C2C12 skeletal myoblasts differentiate toward myotubes even in the absence of differentiation media. 3D printing of the nanocomposite hydrogel is achieved and creation of complex heterogeneous structures that respond to magnetic field is demonstrated. By combining the advanced, stimuli-responsive hydrogel with the architectural control provided by bioprinting technologies, 3D constructs can also be created that, although inspired by nature, express functionalities beyond those of native tissue, which have important application in soft robotics, bioactuators, and bionic devices.