High-quality atomically flat substrates are critical for the analysis and imaging of surface-mounted ultrathin films and nanostructures. Here we report significant improvement in the preparation of large areas of atomically smooth Au(111) substrates. A thin layer of gold on silicon is flame-annealed in air and then stripped from the template. The substrates were analyzed with X-ray diffraction and high-resolution atomic force microscopy (AFM). In contrast to the previously reported template stripped gold (TSG) substrates, flame-annealed template stripped substrates reveal no detectable pinholes. The substrate surface is atomically smooth with most grains being larger than 1 µm 2 . The entire procedure requires less than 2 h and uses readily available materials and common laboratory equipment. The resulting substrates can be stored for longer periods of time and then used immediately without need for common cleaning procedures. Evidence is provided that self-assembled monolayers on these substrates are higher quality than those prepared with previously reported gold substrates.