Helicoidal cellulosic architectures, existing in plant cell walls, were evidenced by Neville in 1976, same year Gray published the first paper related to cellulose based liquid crystalline solutions in vitro. Since then, many works were devoted to cellulose hierarchical helical structures that span from the molecular to the nano, micro, and macroscales. Multifunctional materials were prepared that combine functionality with structural performance. Some examples are chosen to illustrate the rich diversity of cellulose-based materials that are synthetically produced through bioinspired approaches. Main attention will be devoted to cellulose helicoidal out of equilibrium structures and to liquid crystalline cellulose phases as probes for cellulose/water interactions. Future and recent applications will be outlined.