Nanocomposites made of magnetite (Fe3O4) nanoparticles (NP)s with different surface chemistry and Polyvinyl difluoride (PVDF) polymer were investigated using full atom molecular dynamics (MD) simulation. NPs with OH, hexanoic, and oleic acid terminations were considered in this study. The effect of each surface chemistry was investigated in terms of its effect on the mechanical properties, local interaction through the distribution of the internal energy around the NP, and the chain polarization gradient from the interface to the bulk. From this investigation, it appears that the oleic acid although the most popular, is the less favorable for interfacial interaction and local polarization. The OH-terminated NP presents the best configuration for the investigated properties. The hexanoic acid-grafted NP presents a good compromise. The hydrogen bonding appears to govern the induced response of the nanocomposites. Although the hexanoic acid grafted NP presents less hydrogen bonding than the OH one, the conformation of the hexanoic acid acts as a mobility flow inhibitor and therefore leads to comparable performance in comparison to the OH-terminated NP composite. This work led to investigating routes to make materials with well-optimized multiple properties in the case of nanocomposite materials. Such results shed light on the multiple combinations offered by nanocomposites that go beyond the only standard nanosize effects.