Aragonite helical fibers in the shell of a pteropod Cavolinia globulosa are shown to consist of single-crystalline rod-like building blocks ∼1 μm long and ∼100–200 nm wide. Although the building blocks of the orthorhombic crystal share similar c-axis orientations along the surface normal, their a and b directions rotate in a stepwise fashion. The crystallographic rotation of the unit rods and the twisted stacking of the fibers along the helical axis form the specific hierarchical architecture of the pteropod shell.