This work explores the fascinating properties of charged nanocellulose polyelectrolyte hydrogels. By integrating charged nanocellulose with other, natural and synthetic, polyelectrolytes we are able to expand the range of phase behaviors and material assembly pathways, ultimately enriching the resultant properties of these composite hydrogel systems. In this presentation, I will share some of our recent work combining structuring and compartmentalization of hydrogel systems to achieve morphing, actutation and logic functions encoded in the materials themselves. These advancements not only demonstrate the versatility of charged nanocellulose polyelectrolyte hydrogels but also open new avenues for their application in e.g. soft robotics, responsive materials, drug delivery systems and bioengineering.