As a sort of cathode material with appreciable theoretical capacity, sulfur has received a lot of attention for lithium-sulfur batteries. There is extensive research focused on cathode materials. However, relatively little attention has been gained on a binder in enhancing battery performance. The binding agent is a primary component in the cathode and plays an important role in solving the sulfur volume expansion problem during the reaction. In this work, Al (III)-carboxylate metal-organic aerogels (Al-MOGs) are reported for the first time as a binder, which can anchor the diffusion of hydrophilic polysulfides in the cathode and restrain a self-discharge reaction from proceeding for the Li-S battery. In the charge-discharge system, the admirable electrochemical performance of the as-fabricated combination cathode is proven through a satisfactory initial discharge capacity and good rate performance (1391 mAh g(-1) at 0.3 C and 664 mAh g(-1) at 6.0 C) and a notable cyclability (902 mAh g(-1) after 200 cycles at 0.3 C). Accordingly, the creation of Al-MOG gives an updated perception for high-energy-density Li-S batteries.