Post-synthesis methods are a promising technology and have received much attention. In this paper, a series of post-synthesis aluminum modified TUD-1 (PAT) materials with different Al contents were successfully prepared by using aluminum isopropoxide to be Al sources, then the as-synthesized materials were adopted as support additives mixed with commercial γ-Al 2 O 3 to prepare hydrodesulfurization (HDS) catalysts for FCC diesel. The supports and catalysts were analyzed using N 2 adsorption-desorption, XRD, SEM, Py-IR, ICP, 27 Al MAS NMR, UV-vis, H 2 -TPR and HRTEM techniques. The results of Py-IR and 27 Al MAS NMR indicated that the addition of Al species could bring Lewis (L) and Brönsted (B) sites into Si-TUD-1, and that the material of PAT-3 had the highest total acidity sites and Brönsted acid sites among the series PAT composites. The HRTEM technique showed that, compared to the traditional catalyst NiMo/γ-Al 2 O 3 , the sulfided catalyst NiMo/APAT-3 had a relatively short length (3.2 nm) and suitable stacking number (2.5) of MoS 2 slabs. The HDS efficiencies of all the catalysts were tested in a fixed bed micro-reactor with FCC diesel as feedstock. The catalytic results confirmed that the catalyst NiMo/APAT-3 possessed the highest HDS efficiency (97.0%), due to synergistic effects of advantageous properties such as higher acidity, moderate MSI, and relatively short length of the MoS 2 slabs.