Novel raft-like zinc(II)-phenylaianine complexes and zinc(II)-phenylalanine/acid green 27 (AG27) hybrid radial bundles have been successfully synthesized by a simple refluxing reaction. The formation processes of the morphologies and the superstructures of the hybrid bundles were proposed based on the time-dependent evolution process. The AG27 molecules act as both the inclusion compound and the controller of the morphologies and the superstructures of the final hybrid. The combination of the zinc(II)-phenylaianine complex and AG27 leads to distinct optical properties compared with the individual component materials. This approach opens a new and effective way for the fabrication of amino acid/dye hybrid materials with unique optical properties and is expected to allow access to other organic/organic hybrid materials with structural specificity and functional novelty.