Producing self-assembled monolayer on gold with uniform submonolayer coverage can be challenging due to the tendency of the thiol molecules to form islands on the surface. Loosely packed SAMs have recently garnered scientific interest across a broad range of applications, including antifouling materials and micro/nanofluidic devices. In addition, the added conformational freedom of loosely packed SAMs influences surface properties such as wetting, friction, ion transport, and the film's response to an external stimulus such as a change in pH, temperature, or electrical potential. The creation of low-density self-assembled monolayers (LD-SAMs) requires limiting the spontaneous adsorption of the thiols while achieving a uniform, sub-monolayer packing density and often necessitates a sophisticated, multi-step synthesis scheme. We report a simple and systematic approach to uniformly control the nanoscale structure of charged LD-SAMs on gold surfaces. We take advantage of ion-pair chemistry, commonly used in liquid-phase extraction and ion-exchange chromatography applications, to sequester the thiol molecule in a stable ion-pair complex and to create steric hindrance during the SAM depostion. The versatility and simplicity of this approach allows for systematic variation of surface coverage. We have extensively characterized the formation, deposition, and stability of the LD-SAMs using a wide range of techiques (X-ray photoelectron spectroscopy, FT-IR spectroscopy, electrochemical impedance spectroscopy, cyclic voltammetry, and contact angle measurements) to show that the ion-pair complexes form in solution and remain as a complex during the self-assembly process. We also demonstrate that the size of the complex dictates the spacing of the thiol chains. Finally, we demonstrate that the ion-pair complex can be easily broken and released from the surface of the LD-SAM through a simple ion-exchange step.