To enhance dibenzothiophene (DBT) capture performance, we innovatively synthesized a series of novel multimetal-organic frameworks (MMOFs) by the incorporation of Ag+, Cu2+, Zn2+, and Ni2+ within one structure. Those novel desulfurizers have been fully characterized and their structural changes further compared in terms of nitrogen adsorption-desorption, powder X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, inductively coupled plasma, X-ray photoelectron spectroscopy, and so forth. The DBT capture properties with as-synthesized MMOFs in different simulated fuels were evaluated through a series of batch tests. All further investigations demonstrated that the Ag/Zn/Ni/Cu-BTC exhibited a remarkably high sulfur capacity attributed to the associative effects of pi-complexation and acid-base interaction. Additionally, based on sieving and inertia mechanisms, this adsorbent possessed an extremely high affinity for DBT capture in the presence of benzene and octane. Especially, the Ag/Zn/Ni/Cu-BTC could sustain an outstanding desulfurization property after the fifth cycle. Our study opens up a new perspective for the design of desirable MMOF materials, promoting their potential development in the aspects of adsorption desulfurization.