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[Display omitted] • Amorphous Al 2 O 3 in porous carbon anchored on carbon cloth was first fabricated. • The composite was investigated as a multifunctional interlayer for Li-S batteries. • The Li-S cells with high sulfur-loading exhibited superior cycling stability. • The Li-S cells exhibited excellent rate capability. • The amorphous Al 2 O 3 in porous carbon can effectively suppress the LPS shuttle effect. To realize practical applications of lithium-sulfur batteries, rational strategies have to be applied to overcome obstacles such as the shuttle effect and sluggish reaction kinetics of soluble long-chain lithium polysulfides (LPS). In this work, highly electrocatalytic active amorphous Al 2 O 3 uniformly dispersed in porous carbon (Al 2 O 3 /C) anchored on carbon cloth (CC) was successfully fabricated. The resultant flexible Al 2 O 3 /C@CC was used as an independent interlayer for Li-S batteries, demonstrating strong physical confinement and chemical binding ability for LPS, as well as high catalytic activity for LPS conversion kinetics due to a synergistic effect of 3D conductive network, amorphous nature of Al 2 O 3 /C, porous structure and abundant active sites. The cells with such interlayer exhibit high specific capacity, superior cycling stability and rate capability, 903 mAh/g at 0.2C after 100 cycles and 810 mAh/g at 1.0C after 300 cycles can be achieved, moreover, 741 mAh/g can still be retained at a high rate of up to 5.0C. By contrast, Al-MOF grown on carbon cloth (Al-MOF@CC) exhibits limited performance improvement due to poor electrical conductivity, low structure stability, as well as limited ion diffusion rate and weak Lewis acid-base interactions due to lack of open channels. [ABSTRACT FROM AUTHOR]