Especially in the medical, sports tracking, and the virtual reality sectors, the market for reliable, affordable, and sensitive sensors is growing quickly. Commercially available sensors, e.g. chemical sensors based on metal oxides often face problems of low selectivity and high operating temperatures. In contrast, organically capped or cross-linked metal nanoparticle assemblies have shown promising sensing properties at room temperature. Gold nanoparticles (GNPs) are valuable due to their high stability and their well-controlled synthesis. In particular in combination with thiols, GNP assemblies have been used as chemiresistors and as strain sensors. Nowadays, various techniques for their fabrication exist, opening up the opportunity to design well-controlled thin films for different sensing applications.