In the present study, the compressive behavior of polydimethylsiloxane (PDMS)-iron oxide nanocomposites (PIONs), particularly the effects of the iron oxide nanoparticle content and surfactant, was investigated. PIONs have been employed in various micro-and nano-engineering applications due to their advantageous properties. However, characterization of the mechanical characteristics is still insufficient, thereby limiting wide-spread application. In this regard, a compression test was carried out to evaluate the fundamental compressive behavior of the PION. The specimens were prepared by changing the content of the iron oxide filler and by modulating the surface energy of the PDMS matrix using a surfactant. From the stress-strain characteristics, the relationship between the compressive elastic modulus and iron oxide content was found to be linear. In addition, the native PION exhibited around 73.5% greater increase in the normalized compressive elastic modulus than the surfactant-treated PION, showing a negative effect of the increased surface energy.