Brucine inclusion crystals with neutral guest molecules exhibit guest-dependent polymorphism due to a hierarchical structure. Chiral brucine molecules are regarded as a primary structure and assemble to form a chiral tape with a 21 axis as a common secondary structure. Such tapes meet together in various modes to constitute different bundles as a tertiary structure. The bundle modes are theoretically classified into eight types, which were screened by alteration of guest compounds in the volume range from 39 to 150 angstrom(3).