Dynamic Morphological Transformation and Self‐Assembly of DNA‐Functionalized Cellulose Nanocrystal Building Blocks

Self-assembly of cellulose nanocrystals represents one of important pillars of nanoscience that integrates natural design motifs into development for sustainable solutions in key industries. However, there is only a limited number of methods that confer manipulation of interparticle interaction between cellulose nanocrystal building blocks and synthesis of well-defined self-assembly architectures. Herein, a DNA-mediated strategy that enables a dynamic stepwise rod-to-sphere-to-rod morphological transformation of cellulose building blocks is introduced, culminating in the formation of slab-like cellulose architectures in colloidal states. This work establishes a strategic bridge between cellulose nanocrystal assembly and programmable anisotropic nanoparticle systems while addressing a long-standing challenge in DNA nanotechnology to producing scalable, biocompatible micro-scale self-assembly architectures. This work is envisioned that it may galvanize further research that accelerate the development of transformative solutions to address unmet challenges in medicine, energy, and soft robotics, particularly as carriers and scaffolds.