Aluminum-free Ni-incorporated MFI zeolite materials were synthesized in a batch reactor under mild reaction conditions using the hydrothermal method and were proven to exhibit highly active sites for the saturation of aromatics and olefinic molecules due to the high dispersion of the Ni species. The synthesized solid materials were characterized by various methods, and computational modeling aided in understanding the Ni dispersion in the MFI framework. The novelty of this study is corroborated to the unprecedented hydrogenation activity of the Ni-MFI materials when tested with a 1-octene model molecule at 0.48 MPa H-2 pressure and moderate temperatures (423-473 K). Another important aspect of this work is the significant elimination of olefinic molecules from a sulfur-rich industrial cracked naphtha feedstock when using extrudates of the same material, which enforces that Ni-MFI could be commercially applied in industry for the selective hydrogenation of olefins present in light petroleum streams.