Polymerization of carbazole dicarboxaldehydes and lysine derivatives by imine and acylhydrazone formation afforded peptide-derived molecular biodynamers. Characterization of their physicochemical properties revealed an interesting morphology change upon polymerization from monomers forming submicrometer spherical micelles to nanometer-sized rigid-rod-shaped polymeric particles. A combination of light-scattering methods, small-angle neutron scattering, and transmission electron microscopy enabled a detailed investigation of this morphological change. Moreover, we investigated by dynamic and static light scattering how the pH affects the fluorescence and size of the biodynamers. These morphological and pH-dependent changes are expected to open the door to a myriad of applications of molecular biodynamers.