Formation of intended nano-and microstructures with regular building blocks has attracted much attention because of their potential applications in the fields of optics, electronics, and catalysis. Herein, we report a novel strategy to spontaneously grow three-dimensional (3D) hierarchical cabbagelike microparticles (CLMPs) constructed by individual Au nanoplates. By reducing gold precursor to gold atoms, N-(3-amidino)-aniline (NAAN) itself was oxidized to form poly(N- (3-amidino)-aniline) (PNAAN), which specifically binds on Au(111) facet as a capping agent and which leads to the formation of gold nanoplates. Because of the incomplete coverage of Au(111) facet, new gold nanoplate growth sites were spontaneously generated from the crystal plane of existing Au nanoplates for the growth of other nanoplates. This process continued until the nanoplate density reached its maximum range, eventually resulting in CLMPs with well controlled structures. This opens a new avenue to utilize the imperfection during nanoparticle (NP) growth for the construction of microstructures. The individual CLMP shows excellent surface-enhanced Raman scattering (SERS) performance with high enhancement factor (EF) and good reproducibility as it integrates the SERS enhancement effects of individual Au nanoplate and the nanogaps formed by the uniform and hierarchical structures.