Multispiked gold nanoparticles are required in large quantities for many fundamental studies and applications like (bio)sensing, but their preparation in high yield by the bottom-up chemical synthetic method is challenging. A water-based, non-‘seed-mediated’, straightforward method for the synthesis of gold nanoparticles with well-developed surface spikes is reported here. The yield of multispiked gold particles is very high (>90%). The method allows the tuning of the number and size of the spikes and the overall size of the particles, and hence the localized surface plasmon resonances of the particles over the broad spectral range in the visible and near-infrared. A mechanism for the evolution of twinned, sharp-tipped surface protrusions has been proposed based on systematic spectrophotometric and transmission electron microscopic studies, which were employed to elucidate the morphological features, structure, chemical composition, and optical properties of the multispiked gold nanoparticles.