This work describes exploration of mitigating the parasitic amorphous alumina (Al2O3) shell of aluminum nanoparticles (n-Al) and modifying the surface using different plasmas, leading to n-Al with thinner shell and different coatings including carbons and oxidizing salt called aluminum iodate hexahydrate (AIH), respectively. The approach exploits a prototype atmospheric non-thermal plasma reactor with dielectric barrier discharge (DBD) configuration for nanoparticle surface modifications using n-Al of 80 nm average diameter as an example. Preliminary results indicate that the amorphous Al2O3 shell surrounding the active aluminum core can be mitigated with inert plasmas by as much as 40% using either helium (He) or argon (Ar). The particle surface becomes carbon-rich with carbon monoxide (CO) / He plasmas. By immersing the plasma-treated n-Al in an iodic acid (HIO3) solution, AIH crystals can be formed on the n-Al surface. Transmission electron microscopy (TEM) is used as a major tool to study the details of the modified surface morphologies, diffraction patterns, and chemical composition of the modified n-Al. The results demonstrate effective surface passivation of n-Al via atmospheric plasma techniques.