plasticity under compressive stress, suggesting that such deformation can be controlled. [2] However, this material is strongly anisotropic owing to its limited number of slip systems. Micro-or nanostructure design has already been employed in some vdW materials to enhance plasticity, such as BN, which opens a new avenue for large plastic deformation of polycrystalline vdW materials. [3] Achieving large deformation in graphite or graphene by means of microstructure manipulation also attracts researchers' attention. [4][5][6][7] The sp 2 hybridization in graphene layers makes them capable of resisting in-plane stretching and compression, while their ability to bend and fold enables them to sustain large elastic distortions. These features have been demonstrated in carbon nanotubes (CNTs), graphene sheets, and fullerenes. [8] Carbonaceous materials are classified as amorphous carbon and crystalline carbon. Graphite crystallites typically do not grow in amorphous carbon, even after heat treatment at high temperatures. Thus, amorphous carbon Obtaining large plastic deformation in polycrystalline van der Waals (vdW) materials is challenging. Achieving such deformation is especially difficult in graphite because it is highly anisotropic. The development of sugar-derived isotropic nanostructured polycrystalline graphite (SINPG) is discussed herein. The structure of this material preserves the high in-plane rigidity and out-of-plane flexibility of graphene layers and enables prominent plasticity by activating the rotation of nanoscale (5-10 nm) grains. Thus, micrometersized SINPG samples demonstrate enhanced compressive strengths of up to 3.0 GPa and plastic strains of 30-50%. These findings suggest a new pathway for enabling plastic deformation in otherwise brittle vdW materials. This new class of nanostructured carbon materials is suitable for use in a broad range of fields, from semiconductor to aerospace applications.