Living organisms, from the cellular to the body-system level, present elegant designs that realize desirable structures, properties and functions. Tendons and muscles, for example, are tough yet soft thanks to hierarchical structures rarely found in synthetic materials. Our neuromuscular system senses and responds to motion with built-in feedback control, an intelligence manmade systems lack. Gels, liquid-laden crosslinked polymer networks, have tissue-like water-rich porous structures and change their volume and properties in response to environmental cues. At the UCLA He lab, we study processing-structure-property-function relationships of hydrogels and their derivatives to create (i) 'bio-like' structures and properties and (ii) 'life-like' intelligence in soft materials for robotics, biomedicine, energy and environment. This talk will show how mastering polymer-water interactions through physical processing makes this possible. Using classic chemical physical principles to modulate macromolecule assembly into complex networks, we can break fundamental limits in mechanical, diffusion and electrical properties. Three handles will be discussed: thermodynamically, ions and cosolvents drive chain aggregation; kinetically, chain mobility and processing sequence set when the structure locks in; spatially, directional freezing and temperature gradients direct where it forms, programming hierarchy across length scales. With feedback and time delay built into the material itself, responsive gels and elastomers track, oscillate and roll autonomously. The resulting soft materials, combining high toughness, ion/electron conduction, fast response and 'synthetic intelligence,' enable energy-self-sufficient robots, personalized medical implants, smart wearable electronics and battery-powered flight.