Layered materials, being a source of 2D systems, have undergone a renaissance in the past years as they provide a rich playground for studying structure-property relationships on going from three to two dimensions. The talk will highlight our recent progress in the development of "soft" 2D systems –– carbon nitrides and covalent organic frameworks –– which show potential as abundant and molecularly tunable organic semiconductors for solar hydrogen evolution. The second part will give an outlook on our activities in developing new ultrafast lithium solid electrolytes from layered sulfides and thiophosphates, and in studying their lithium ion dynamics in the solid state.