The epoxide addition sol-gel method has been utilized to synthesize porous zinc-copper composite aerogels in the zinc-to-copper molar ratios of 50: 50 to 90: 10. A two-step mixing approach has been employed to produce aerogels composed of nano- to micrometer sized particles. The aerogels were characterized by ultrahigh resolution scanning electron microscopy, transmission electron microscopy, and powder X-ray diffraction. The as-synthesized aerogels had a thin flake- or petal-like microstructure comprised of clustered flakes on two size scales; they were identified as being crystalline with the crystalline species identified as copper nitrate hydroxide, zinc hydroxide chloride hydrate, and zinc hydroxide nitrate hydrate. Annealing of the aerogel materials at a relatively low temperature (400°C) resulted in a complete phase transition of the material to give highly crystalline ZnO-CuO aerogels; the aerogels consisted of networked nanoparticles in the 25-550 nm size range with an average crystallite size of 3 nm and average crystallinity of 98%. ZnO-CuO aerogels are of particular interest due to their particular catalytic and sensing properties. This work emphasizes the versatility of this sol-gel route in synthesizing aerogels; this method offers a possible route for the fabrication of aerogels of different metal oxides and their composites.