Carboranes that have a high boron content are key materials for boron neutron capture therapy (BNCT), while PEGylated gold nanoparticles (AuNPs) are also most useful in various aspects of nanomedicine including photothermotherapy, imaging and drug vectorization. Therefore, methods to assemble these key components have been investigated for the first time. Strategies and results are delineated in this article, and the nanomaterials have been characterized using transmission electron microscopy (TEM), dynamic light scattering (DLS), UV-vis., mass and multinuclear NMR data. A series of well-defined water-soluble bifunctional AuNPs containing carborane and polyethylene glycol (PEG) were synthesized through either two-step Cu(I)-catalyzed azide-alkyne cycloaddition CuAAC ("click") reactions at the periphery of azido-terminated AuNPs in the presence of the efficient catalyst [Cu(I)tren(CH2Ph)(6)][Br] or simply by direct stabilization of AuNPs using a tris-carborane thiol dendron or a hybrid dendron containing both PEG and carborane.