Optimal ink formulations, inclusive of nanoparticles, are often limited to matching the nanoparticles capping agent or surface degree of polarity to the solvent of choice. Rather than relying on this single attribute, nanoparticle dispersibility was optimized by identifying the Hansen solubility parameters (HSPs) of decanoic-acid-capped 5 nm silver nanoparticles (AgNPs) by broad spectrum dispersion testing and a more specific binary solvent gradient dispersion method. From the HSPs, solvents were chosen to disperse poly(methyl methacrylate) (PMMA) and nanoparticles, give uniform evaporation profiles, and yield a phase-separated microstructure of nanoparticles on PMMA via film formation by solvent evaporation. The goal of this research was to yield a film that is reflective or transparent depending on the angle of incident light (i.e., optically variable). The nanoparticle HSPs were very close to alkanes with added small polar and hydrogen-bonding components. This led to two ink formulations: one of 90:10 vol % toluene/methyl benzoate and one containing 80:10:10 vol % toluene/p-xylene/mesitylene, both of which yielded the desired final microstructure of a nanoparticle layer on a PMMA film. This approach to nanoparticle ink formulation allows one to obtain an ink that has desirable dispersive qualities, rheology, and evaporation to give a desired printed structure.