Firstly, the self-assembled morphologies of SVAs in the presence of NPG were investigated. Figures show the TEM micrographs of self-assembled SVAs doped with NPG, in which the dark regions represent the P4VP domains. It is found that the introducing of NPG can effectively regulate the intrinsic morphology of SVA. With the increasing of doping concentration, the self-assembled structures of SVA gradually transfer from cylinder to lamellar. Interestingly, as the doping concentration of NPG is below 10%, self-assembled nanostructures with isotropic morphology can be observed, e.g., SVA/N5 (Figure ). To achieve a statistical description on the TEM microscope, their fast Fourier transform (FFT) patterns were analyzed. For SVA/N5 and SVA/N10, ring-like FFT patterns can be observed. In contrast, the FFT pattern of SVA/N20 shows hexagonally arranged spots, and highly aligned spots can be obtained from the TEM microscope of SVA/N40, due to the oriented textures on TEM micrographs (see more details in SI, Figure ). These results are consistent with the TEM real-space observation. Again, it suggests that continuous but disordered nanostructures can be self-assembled by SVA in the presence of NPG at certain concentration. According to TEM and SEM observation, the phase diagram of SVA/NPG can be determined as shown in Figure .