PVA/SWNT dispersions yield aloe plant‐like crystals, where the leaves are single crystals templated by PVA coated SWNT. Longer growth times (≈18 months) lead to hexagonal rod‐like crystals. HR‐TEM images show evidence that PVA molecules are aligned parallel to the SWNT axis. WAXD, electron diffraction, and HR‐TEM observations of these aloe plant and hexagonal crystals suggests evidence for possible PVA‐SWNT epitaxy. Wide‐angle and electron diffraction data of these crystals also show that the structure seems to mimic the 2D hexagonal crystal packing of SWNT. PVA lattice images and moiré fringes were also observed in the leaf‐like crystals.