We have developed an apparatus that allows the observation of the transient rotational motion of fine particles under a high magnetic field in order to determine anisotropic magnetic susceptibility. The anisotropic susceptibilities of spherical nanoparticles of bismuth and commercially available carbon nanofibers were determined. The estimated Δχ = 3.9 × 10−5 of spherical bismuth nanoparticles with a diameter of 370 nm was fairly consistent with the value determined previously by the magnetic field dependence of diffraction peak intensity in the X-ray diffraction (XRD) pattern, but was slightly smaller than the value for the bulk crystal. In contrast, the transient behavior of carbon nanofibers did not obey the theoretical motion of a single crystal. The wide distribution of fiber lengths, the irregularity of the structure in the fiber, and the connections between the fibers are suggested for the anomalous behavior.