Three-dimensional (3D) morphological evolution and growth mechanisms of primary I-phase particles have been investigated in directionally solidified Al–6Mn–2.5Be (wt%) alloy at a wide range of growth rates (100–1500 μm/s). At relatively low growth rates (100–600 μm/s), the I-phase particles exhibit faceted growth with strong anisotropy, forming a hierarchical flower-like aggregate with icosahedral morphological symmetry composed of several attached irregular polyhedrons or pentagonal dodecahedrons. At higher growth rates (e.g., 1000 μm/s), the interface of the I-phases becomes unstable along the edges and corners of the pentagonal dodecahedron, thereby arousing growth perturbations. Correspondingly, a transition from faceted to nonfaceted growth occurs with increasing growth rate. Further increase of the growth rate leads to the formation of I-phase columnar dendrites' preferential growth along the 3-fold axis. The configurations of the flower-like aggregates can be adequately illustrated by a geometrical model in terms of the perfect and elongated pentagonal dodecahedrons. A growth mechanism for the flower-like aggregates has been proposed based on the clear understanding of the 3D morphological evolution of the I-phase particles.