As with many other bio-sourced colloids, chitin nanocrystals (ChNCs) can form liquid crystalline phases with chiral nematic ordering. In this work, we demonstrate that it is possible to finely tune the liquid crystalline behavior of aqueous ChNC suspensions. Such control was made possible by carefully studying how the hydrolysis conditions and suspension treatments affect the colloidal and self-assembly properties of ChNCs. Specifically, we systematically investigate the effects of duration and acidity of chitin hydrolysis required to extract ChNCs, as well as the effects of the tip sonication energy input, degree of acetylation, pH and ionic strength. Finally, we show that by controlled water evaporation, it is possible to retain and control the helicoidal ordering in dry films, leading to hierarchical architecture analogous to that found in nature, e.g. in crab shells. We believe that this work serves as a comprehensive insight into ChNC preparation and handling which is required to unlock the full potential of this material in both a scientific and industrial context.