Conventional hydrodesulfurization (HDS) to convert the sulfur compounds into sulfide was Co-Ni-Mo/Al2O3 or Ni-W/Al2O3 with impregnation method. Impregnation has its shortcomings. It easily leads to the uneven loading and loss of active ingredient. HTLCs as catalyst precursors can be in formation of metal oxides and metal when they are calcined and reduced. It can be noted that the metal oxides and metal derived from HTLCs have a large surface area, well metal particles dispersion, redox and acid-base characteristics, which are good catalysts in catalysis fields. These properties of the metal oxides and metal derived from HTLCs described by literature are well in line with hydrodesulfurization (HDS) catalyst. This article is mainly about HTLCs as a precursor to hydrodesulfurization. We synthesized binary Ni-Al-HT with interlayer CO32- anions and conducted a preliminary study on the desulfurization of Ni-Al-HT as a precursor. The precursors of hydrogen-like structures of Ni-Al-HT catalysts with different Ni/Al ratios have been synthesized by co-precipitation method. The precursors were reduced at about 500oC to get the catalysts. The hydro-desulfurization activity measurements are evaluated at different conditions (temperature, pressure, volume space velocity, H2/oil ratio) in 10 ml catalyst evaluation device. The physic-chemical characteristics of catalysts precursors and catalysts are obtained using X-ray diffraction (XRD), temperature programmed reduction (TPR), Thermal Gravity Analysis (TG) and Differential Thermal Gravity Analyses (DTG) and FT-IR spectra. The XRD patterns and the FT-IR spectra of Ni-Al-HT with different molar ratio confirmed the successful synthesis of catalyst precursors. The reduced Ni-Al2O3-HT was confirmed in the XRD patterns of Ni-Al2O3-HT. The results of catalytic activity measurements showed that the catalysts with HTLCs as precursors have high hydro-desulfurization yield, hydrogen-like precursors have good prospects.