Effective synthesis of anisotropic nano-/microparticles (APs) by the copolymers is of great significance in nanomaterials and nanotechnology. However, achieving regulation of the morphology, composition, property, and particle size of anisotropic nano-/microparticles (APs) with diversified copolymers is difficult due to complex mechanism and formation conditions. In this work, a versatile one-pot solvent-mediated self-assembly (SmSa) strategy had been proposed for the facile one-pot synthesis of shape-tunable anisotropic nano-/microparticles (StAPs). In addition, the formation mechanism of StAPs was determined through numerous characterization methods related to morphology and element distribution. The results revealed that the anisotropic architectures of StAPs were closely related to the nature of poly(methylacrylic acid-methyl methacrylate-butyl acrylate) (L-1) and poly(butyl acrylate-styrene) (L-2) polymer chains imparted by polymer blocks of different domains. Therefore, the ordered assembly of the rigid and hydrophobic L-2 polymer chains in micelles consisting of the flexible and amphiphilic L-1 and solvent could be successfully carried out under the mediation of increasing solvent polarity and the strong adsorption of poly(vinylpyrrolidone) for L-2. Furthermore, the developed versatile SmSa strategy and the obtained StAPs play an essential role in the development of nanoscience and nanotechnology. Particularly given its adjustable emulsifying properties at different pH values, as well as numerous sites for further modification by fluorescent or other components, it can be employed to synthesize a wide range of functional materials.