The advent of conductive self-healing (CSH) hydrogels, a class of novel materials mimicking human skin, may change the trajectory of the industrial process because of their potential applications in soft robots, biomimetic prostheses, and health-monitoring systems. Here, the development of a mechanically and electrically self-healing hydrogel based on physically and chemically cross-linked networks is reported. The autonomous intrinsic self-healing of the hydrogel is attained through dynamic ionic interactions between carboxylic groups of poly(acrylic acid) and ferric ions. A covalent cross-linking is used to support the mechanical structure of the hydrogel. Establishing a fair balance between the chemical and physical cross-linking networks together with the conductive nanostructure of polypyrrole networks leads to a double network hydrogel with bulk conductivity, mechanical and electrical self-healing properties (100% mechanical recovery in 2 min), ultrastretchability (1500%), and pressure sensitivity. The practical potential of CSH hydrogels is further revealed by their application in human motion detection and their 3D-printing performance.

Strong, stretchable, and durable biomaterials with shape memory properties can be useful in different biomedical devices, tissue engineering, and soft robotics. However, it is challenging to combine these features. Semi‐crystalline polyvinyl alcohol (PVA) has been used to make hydrogels by conventional methods such as freeze–thaw and chemical crosslinking, but it is formidable to produce strong materials with adjustable properties. Herein, a method to induce crystallinity and produce physically crosslinked PVA hydrogels via applying high‐concentration sodium hydroxide into dense PVA polymer is introduced. Such a strategy enables the production of physically crosslinked PVA biomaterial with high mechanical properties, low water content, resistance to injury, and shape memory properties. It is also found that the developed PVA hydrogel can recover 90% of plastic deformation due to extension upon supplying water, providing a strong contraction force sufficiently to lift objects 1100 times more than their weight. Cytocompatibility, antifouling property, hemocompatibility, and biocompatibility are also demonstrated in vitro and in vivo. The fabrication methods of PVA‐based catheters, injectable electronics, and microfluidic devices are demonstrated. This gelation approach enables both layer‐by‐layer and 3D printing fabrications.

Presented in this work is a novel and facile approach to fabricate an elastic, attachable, and cost-efficient carbon nanotube (CNT)-based strain gauge which can be efficiently used as bodily motion sensors. An innovative and unique method is introduced to align CNTs without external excitations or any complicated procedure. In this design, CNTs are aligned and distributed uniformly on the entire chewing gum by multiple stretching and folding technique. The current sensor is demonstrated to be a linear strain sensor for at least strains up to 200% and can detect strains as high as 530% with a high sensitivity ranging from 12 to 25 and high durability. The gum sensor has been used as bodily motion sensors, and outstanding results are achieved; the sensitivity is quite high, capable of tracing slow breathing. Since the gum sensor can be patterned into various forms, it has wide applications in miniaturized sensors and biochips. Interestingly, we revealed that our gum sensor has the ability to monitor humidity changes with high sensitivity and fast resistance response capable of monitoring human breathing.