The free electrons inside precious metals such as Au vibrate when the surface of the metal is irradiated with an electromagnetic wave of an appropriate frequency. This oscillation is referred to as surface plasmon resonance (SPR), and the resonance frequency varies with permittivity of the medium around the metal. SPR sensors are widely applied in the fields of bioscience and pharmaceutical sciences, including biosensing for drug discovery, biomarker screening, virus detection, and testing for food safety. Here, we fabricated a metal-insulator-metal (MIM) SPR sensor by constructing two-dimensional (2D) regular array of Au colloidal particles (2D colloidal crystals) on an insulator layer over a thin Au film coated on a glass substrate surface. The 2D crystals were fabricated by electrostatically adsorbing negatively charged three-dimensional crystals onto a positively charged thin insulator formed on Au film. The plasmon peaks/dips from the MIM structure were measured in aqueous solutions of ethylene glycol (EG) at various concentrations. Multiple plasmon peaks/dips were observed due to the localized SPR (LSPR) of the Au particles and the Fano resonance between the Au particles and thin film. The plasmon peaks/dips shifted to higher wavelengths on increasing EG concentrations due to an increase in the refractive index of the media. The observed peak/dip shift was approximately twice that of LSPR from an isolated Au particle. We expect the present MIM substrate will be useful as a highly sensitive sensor in the pharmaceutical field.