As nanotechnology has developed, the creation of nanostructured surfaces has garnered attention for their uses in sensing and catalysis applications. These are however often expensive, time-consuming, and difficult to produce. In contrast, this investigation is focused on the inexpensive, environmentally friendly and fast technique of Confined Atmospheric Pulsed laser deposition (CAP). The CAP technique has these advantages because it is an atmospheric laser-based direct deposition technique. Herein, the CAP process is examined in an effort to better understand the process and to begin determining the means to control the properties of the nanostructured surfaces produced by varying the laser fluence and the scan strategy during the ablation. During this investigation, a Nd:YAG laser was applied to deposit gold nanostructures directly onto a polymer substrate. The plasmonic properties and morphologies of the surfaces were examined using UV–Vis spectroscopy and Scanning Electron Microscopy (SEM) respectively. A mathematical model was developed to describe the size and dispersity of the structures deposited and the variation of the position and size of the spectral plasmon peaks in response to the sample processing parameters, with the aim of allowing for a degree of control over these properties and gaining some understanding of the mechanism of this deposition process.