Plasmonic nanocrystals, which exhibit extraordinary optical properties, are challenging to grow in selective positions with a cost-effective and high-throughput process. We demonstrate that plasmonic isotropic gold nanospheres (AuNSs) can be selectively synthesized on wafer-scale rigid and flexible substrates at room temperature by laser irradiation. First, we prepare a gold nanocolumnar (AuNC) on sapphire and polydimethylsiloxane substrates by glancing angle deposition (GAD).