In our previous work we demonstrated an unusual crystallite aggregate in which the crystallites correlate in crystallographic orientation and form a fractal pattern with strong anisotropy (Wang, M.; et al. Phys. Rev. Lett. 1998, 80, 3089. Liu, X. Y.; et al. J. Cryst. Growth 2000, 208, 687.). Yet it remains unanswered why each crystallite appears with specific orientation and obeys a strict order. Here we report an in-depth study of the origin of the long-range correlation of the crystallographic orientations in the aggregate investigated by means of micro-X-ray-diffraction, atomic force microscopy, and in-situ optical observation. The experimental data suggest that the topographic regularity of the aggregate arises from the consecutive rotation of the crystallographic orientation in the nucleation-mediated growth. This effect may occur when nucleation takes place in a region with inhomogeneous surface tension, and may help us to understand the long-range ordering effect in aggregating crystallites.