Well-defined gold nanobelts as well as unique gold nanocombs made of nanobelts were readily synthesized by the reduction of HAuCl4 with ascorbic acid in aqueous mixed solutions of the cationic surfactant cetyltrimethylammonium bromide (CTAB) and the anionic surfactant sodium dodecylsulfonate (SDSn). Single-crystalline gold nanobelts grown along the < 110 > and < 211 > directions were prepared in mixed CTAB-SDSn solutions at 4 and 27 degrees C, respectively. Furthermore, single-crystalline gold nanocombs consisting of a < 110 >-oriented stem nanobelt and numerous < 211 >-oriented nanobelts grown perpendicularly on one side of the stem were fabricated by a two-step process with temperature changing from 4 to 27 degrees C. It was proposed that the mixed cationic-anionic surfactants exerted a subtle control on the growth of gold nanocrystals in solution due to the cooperative effect of mixed surfactants. This synthetic strategy may open a new route for the mild fabrication and hierarchical assembly of metal nanobelts in solution. The obtained gold nanobelts showed good electrocatalytic activity toward the oxidation of methanol in alkaline solution; in particular, the electrode modified with the nanobelts obtained at 27 degrees C exhibited an electrocatalytic activity considerably higher than normal polycrystalline gold electrode. Moreover, the gold nanobelts were used as the surface-enhanced Raman scattering (SERS) substrate for detecting the enhanced Raman spectra of p-aminothiophenol (PATP) molecules, and the gold nanobelts obtained at 4 degrees C exhibited an unusual larger enhancement of the b(2) modes relative to the a, modes for the adsorbed PATP molecules.