Metal nanoparticles (Au, Ag, or Pd) functionalized with hydroxy‐terminated alkane thiols can be dispersed in sol–gel mixtures to give alcogels and, after supercritical drying, aerogels containing up to 90 wt% of nanoparticles. Layered or patterned nanoparticle/aerogel monoliths can be prepared by sequential casting or molding of the sol–gels.