An electroless deposition method comprised of seed formation and subsequent seeded growth is developed for the decoration of surface-grown single-walled carbon nanotubes (SWCNTs) with gold nanoparticles of controlled size and interparticle distance. The density of the gold nanoparticles is determined by the density of seeds. Gold seeds are used for the SWCNT arrays grown on SiOx/Si substrates. For the dense SWCNT arrays on quartz, palladium seeds are used because it is much easier to obtain higher quantities of seeds. Attributed to both the seed formation specified on SWCNTs and the succedent efficient seeded growth process, the gold nanoparticles deposit on SWCNTs with very high selectivity. This electroless method shows no selectivity on types, defects, and conductivity of the SWCNTs, and thus ensures the uniform decoration of all SWCNTs on the wafer. Most importantly, this method provides the possibility to realize the optimal configurations of gold nanoparticles on SWCNTs for obtaining maximal surface-enhanced effects and consequently surface-enhanced Raman spectrum (SERS) of each SWCNT. Thus, both the in situ Raman detection of every SWCNT including those nonresonant with laser energy and the observation of the radial breathing modes of SWCNTs originally undetectable with resonance Raman spectroscopy are achieved. Further investigations over the effect of the laser wavelength and the interparticle distance on the SERS enhancement factors of SWCNTs prove that the coupled surface plasmon resonance absorption of the high-density gold nanoparticles decorated on SWCNTs contributes most to the strong surface enhancement.