From the cellular level up to the body system level, living organisms present elegant designs and strategies to realize the desirable structures, properties and functions. For example, tendons and muscles are tough but soft, owing to highly complex hierarchical structures rarely found in synthetic materials. Plants can automatically track the sun and our body can self-regulate motions adaptively to environment, presenting superior intelligence also lacking in manmade systems. Hydrogels, as a class of crosslinked polymers, not only have tissue-like water-rich porous networks and can also change their volume and physical properties in response to environmental cues including temperature, light, and specific molecules. At UCLA He lab, we exploit fundamental material processing-structure-property-function studies of hydrogels and their derivatives, to create (i) ‘bio-like’ structures and properties and (ii) ‘life-like’ intelligence in functional soft materials for applications in robotics, biomedicine, energy and environment. In this talk, I will start with showcasing how the stimuli-responsiveness of hydrogels can unify sensing-diagnosis-actuation process to create ‘synthetic intelligence’ with built-in feedback loop, such as sunflower-like light tracking for solar harvesting (Nat. Nanotech. 2019) and self-sensing actuators for autonomous soft robotics (Sci. Robotics 2019, 2021; Matter 2021). Driven by the remaining challenges revealed in these function developments, I will then present our structural material approaches to breaking the fundamental limits in mechanical, diffusion and electrical properties. I will discuss the mechanics and general principles to design extreme properties, including simultaneously high toughness and stretchability (Nature 2021; Adv. Mater. 2021; Sci. Adv. 2020), tunable porosity and diffusivity (Adv. Mater. 2021; EcoMat 2021) and stretchable conductive soft materials for flexible (bio)electronics (Matter, 2020; Adv. Funct. Mater. 2020; Adv. Mater. 2019). I will conclude my talk with a perspective on future human-machine convergence enabled by soft materials.