The rotation of fullerene chains in SWNT peapods is studied using low-voltage high resolution transmission electron microscopy. Anisotropic fullerene chain structures (i.e., C300) are formed in situ in carbon nanopeapods via electron beam induced coalescence of individual fullerenes (i.e., C60). A low electron accelerating voltage of 80 kV is used to prevent damage to the SWNT. The large asymmetric C300 fullerene structure exhibits translational motion inside the SWNT and unique corkscrew like rotation motion. Another asymmetric fullerene chain containing mixed fullerene species is prepared by fusing smaller C60 fullerenes to a larger Sc@C82 fullerene, and this also exhibits corkscrew rotational motion. Chains of Sc3C2@C80 in SWNT peapods adopt a zigzag packing structure, and the entire zigzag chain rotates inside the SWNT to induce structural modifications to the SWNT diameter and cross-sectional shape of the SWNT. The expansion and contraction of the diameter of the SWNT is measured as 17%, demonstrating nanoactuation behavior in carbon nanopeapods.