The modulation of nanoparticles’ size, shape, and dispersion by polymers has attracted particular attention in different fields. Nevertheless, there is a lack of information regarding the use of charged macromolecules as assistants in the nanostructures’ nucleation and growth processes. Prompted by this, the in situ synthesis of gold nanoparticles (AuNPs) aided by hydrolyzed polyacrylamides (HPAM), with different chemical structures, was developed. In contrast to the conventional synthesis of nanostructures assisted by polyacrylamide, here, the polymerization, hydrolysis, and nanostructure formation processes were carried out simultaneously in the same milieu. Likewise, the growing chains acted as a template for the nanoparticles’ growth, so their conformations and chemical structure, especially the amount of charges along the chain, played an important role in the AuNPs’ morphology, size, and some of the final composite features. The nanocomposite was thoroughly characterized with appropriate techniques, including ATR–FTIR, GPC, UV–Vis, and SEM.