This letter presents a straightforward and economic strategy to create aqueous Au nanoparticle dispersions using small amounts of β-d-glucose as a “green” alternative to the conventional phase-transfer catalyst approach. Furthermore, this new process provides for efficient extraction of these monodisperse Au nanoparticles into an organic phase that was successfully processed into wide-area, locally ordered nanoparticle arrays and thin films using a precisely controlled CO₂-expanded liquid particle deposition technique. This CO₂-based technique allows for pressure-tunable particle deposition while eliminating the detrimental surface tension and dewetting effects common to normal solvent-evaporation techniques.