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In this work, we report a rational design and facile synthetic process for the construction of a 3-dimensional N, S co-doped reduced holey graphene oxide/carbonized cellulose paper as interlayer in Li–S batteries. The interlayer has a labyrinth-like structure with plenty of nanosized holes to achieve the permselectivity for Li ions and effective intercept for polysulfides. The coin cell with the interlayer shows a high initial discharge capacity of 1263.5 mAh/g at 0.2 C, a low capacity fading rate of 0.0487% per cycle for 300 cycles at 1 C, and an excellent rate performance of 864.6 mAh/g at 2 C. Moreover, this cell also has excellent anti-self-discharge property and a high areal capacity of 6.1 mA h/cm2 at a sulfur loading of 8.1 mg/cm2 using aluminum foil as the current collector. Thus, this work suggests the permselective and multifunctional interlayer as a practical and effective strategy for the application in the high-performance Li–S battery. The labyrinth-like N and S co-doped reduced holey graphene oxide/carbonized cellulose paper, as the interlayer of lithium-sulfur batteries, achieved the excellent permselectivity toward Li ions and effective intercept toward polysulfides and exhibited significant cycle stability, anti-self-discharge property and a high areal capacity. Image 1 • A labyrinth-like NS-RHGO-CCP was constructed as interlayer for Li–S batteries. • The NS-RHGO-CCP possessed high permselectivity of Li+ to raise rate capability. • The NS-RHGO-CCP achieved interception of polysulfides to enhance cycle stability. • The NS-RHGO-CCP improved conductivity of S and Li 2 S to give a high areal capacity. [ABSTRACT FROM AUTHOR]