This article introduces a facile nanoparticle self-assembly/annealing method for the preparation of nanoisland films. First, nanoparticle-polymer multilayer films are prepared with layer-by-layer assembly. Nanoparticle multilayer films are then annealed at $~500^{circ}C$ in air to evaporate organic matters from the films. During the annealing process, the nanoparticles on the solid surface undergo nucleation and coalescence, resulting in the formation of nanostructured gold island arrays. By controlling the overall thickness (number of layers) of nanoparticle multilayer films, nanoisland films with various island density and different average sizes are obtained. The surface property of gold nanoisland films is further controlled by the self-assembly of alkanethiols, which results in an increased surface hydrophobicity of the films. The structure and characteristics of these nanoisland film arrays are found to be quite comparable to those of nanoisland films prepared by vacuum evaporation method. However, this self-assembly/annealing protocol is simple and requires only common laboratory supplies and equipment for the entire preparation process.