As schematically represented in Figure , as the volume of TALH precursor solution increases, the zeta potential of the suspension at pH 6 changes from positive to approximately zero and eventually to negative. When the zeta potential is positive/negative, the net positive/negative charge results in electrostatic repulsion. It is clear that as the zeta potential changes from positive to zero, the SP size increases from small SP (Figure ) and reaches a maximum close to zero as observed in Figure . With further decrease of the zeta potential to negative values, the SP size again decreases (Figure ). As the net surface charge decreases, the repulsion is also decreased and results in attractive forces between the negatively charged Au@polymer nanoparticle and positively charged TALH. Therefore, the nanoparticles interact with TALH and start forming SPs. As the zeta potential is close to zero, we consequently observe clustering of nanoparticles, leading to the formation of large SPs. The successful synthesis of these SPs was confirmed by correlating the zeta potential changes with the observed structural evolution, as studied through various electron microscopy techniques. The structural characterization of the synthesized SPs is crucial for understanding the interplay between surface charges and particle assembly, and this relationship is clearly observed in the electron microscopy images discussed below.