Resorcinol based reduction and capping of ultra-small colloidal silvernanoparticles (Ag NPs) optimally formed hydrogen bond driven clusterswithin the water-based solution. Large-area self-assembled fractalstructures of Ag NPs aggregates were fabricated by solvent evaporationtechnique on silicon substrate. The final dried surface structures werefound to be pH dependent which was adjusted to particular values afterthe optimal reduction of silver salt, capping of Ag NPs, followed bycluster formation at an optimum pH in the solution phase. These self-assembled surface structures show controlled enhancement of varioussurface optical phenomena such as Raman spectra of a model dye andluminescence of Ag NPs as a function of pH dependent fractal dimensionof the resulting structures. The structure, morphology and variousrelevant optical properties of self-assembled fractals of Ag NPs werefurther established by combined use of X-Ray diffractometry (XRD),Scanning Electron Microscopy (SEM), Transmission Electron Microscopy(TEM), UV-Visible, photoluminescence and Raman spectroscopy analysis.