The liquid–air interface is demonstrated as a method to assemble nanoparticles synthesized from the reaction between iron (III) dibenzoylmethane (Fe(dbm)3) and platinum acetylacetonate (Pt(acac)2) into a long range monolayer. These surface-modified particles have average Fe to Pt atomic ratio of 0.77:1. The increase in surfactants further reduces the Fe:Pt ratio and increases the particle diameter to over 4 nm. The self-assembled pattern of FePt-based nanoparticles can be enhanced by dropping nanoparticle suspensions on the surface of diethelyne glycol (DEG). The concentrations of these nanoparticle suspensions in hexane from 0.2 to 0.4 mg/ml can be used without the agglomeration into multilayered islands. The voids in the self-assembled monolayer on the DEG-air interface are reduced to the minimum in the case of the lowest concentration.