Nanocrystalline silver dressings are widely known to be potent antimicrobial and anti-inflammatory agents and have long been used to treat topical wounds. Gold is known to be a strong anti-inflammatory agent and has been used in the treatment of rheumatoid arthritis for >70 years. The purpose of this work was to study the effect of incorporating gold into nanocrystalline silver dressings from antimicrobial and anti-inflammatory perspectives. Gold and silver dressing alloys were created by direct current magnetron sputtering and compared with pure silver nanocrystalline dressings using conventional biological (log reduction and corrected zone of inhibition) and physical (X-ray diffraction, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy, atomic absorption spectroscopy, atomic force microscopy and scanning electron microscopy) characterisation techniques. While the gold/silver dressings were slightly weaker antimicrobials than the pure silver nanocrystalline structures, the addition of gold to the nanostructure reduces the minimum crystallite size from 17 to 4 nm. This difference increases the number of grain boundary atoms from 12% to 40% which could augment the anti-inflammatory properties of the dressings. The formation of gold oxide (Au2O3) was thought to be responsible for the observed decrease in crystallite size.