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A metal–oxide–semiconductor (MOS) capacitor embedded with gold nanoparticles (Au NPs) has been successfully fabricated by a spin-coating-derived chemical solution process. The colloidal synthesized Au NPs (∼3.5 nm) were self-assembled to 3-aminopropyltrimethoxysilane-modified silicon oxide substrates. With the spin-coating process, Au NPs can be fabricated onto silicon oxide with a high packing density of 1.6 × 1012 cm−2 in a short processing time. The sol–gel-derived HfO2 layer, acting as a control oxide, was also spin coated to construct an Si/SiO2/Au NPs/HfO2 structure. This MOS structure showed good memory effect and retention properties. This study indicates that it is appropriate to utilize the spin-coating process in nanocrystal memory applications.