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A series of porous metal–organic frameworks (MOFs) of the UiO-66 family, namely UiO-66(Zr), UiO-66(Hf) and UiO-66(Hf)-NH2, prepared by solvothermal procedures were characterized, and their catalytic efficiency for oxidative denitrification (ODN) was investigated for the first time. Sustainable denitrogenation systems combining adsorption and oxidative catalytic capacity were designed using a model diesel containing two distinct nitrogen compounds (NCs) in a solvent-free medium and using an environment-friendly oxidant (H2O2). An efficient adsorptive denitrogenation process was only achieved after long reaction times (24 h): using the Hf-based MOFs, the adsorptive denitrogenation increased from 19% to 79% at 5 to 24 h, while the UiO-66(Zr) reached 76% after 24 h, although the absence of adsorption capacity after 5 h. UiO-66(Hf) and UiO-66(Hf)-NH2 also revealed superior oxidative catalytic denitrogenation than UiO-66(Zr), attaining 97% of efficiency instead of 80%. ODN processes demonstrated to be more effective than the adsorptive denitrogenation, mainly during the first hours of the process. In addition, the metal center in the MOF structure had a larger influence than the presence of the amine-functional groups. Hf-based compounds revealed higher denitrogenation efficiency than the UiO-66(Zr) for a shorter reaction time (5 h).