. The focus of this work is on the functionalization of gold nanoparticles, GNPs, with doxorubicin, D, an anticancer drug, both in the absence and in the presence of natural adjuvant biomolecules, like piperine, P, resveratrol, R, resveratrol-piperine, RP, complex, and icariin, I, which are therapeutic molecules with demonstrated anticancer and anti-inflammatory activity, to form highly stabilized colloidal dispersions. The green syntheses of GNPs, as cores, loading self-assemblies of various selected biomolecules, adsorbed on their surface, as shells, was confirmed by observing surface plasmon resonance at about 538 nm. Further, gold nanoparticles stabilized by resveratrol, GNP-R, are functionalized with various concentrations of selected biomolecules: D, P, R, RP, and I, resulting in different D/P/R/RP/I@GNPs-R composite nanoparticles for various compositions. Another series of stabilized colloidal dispersions is generated as GNP-R1, where the initial GNP-R is centrifuged and washed and then it is dispersed in aqueous solutions and further functionalized with said selected biomolecules. This study proves the functionalization of GNPs, as composite nanoparticles of high stability, in the presence of phosphate buffer saline, PBS, as confirmed by UV-Vis spectra of their colloidal aqueous dispersions.