Lithium-sulfur batteriess tands out as ap romising technology for energy storageowing to acombination of favorablec haracteristics includingahight heoreticalg ravimetric capacity,e nergy density,i nexpensive character,a nd environmental benignity.C ovalento rganic frameworks (COFs) are ar apidlyd eveloping family of functional nanostructures which combinep orosity and crystallinity,a nd whichh ave been already used in these kinds of batteries to build sulfur electrodes, by embedding sulfur into porous COFs in order to enhancec ycle lifetimes. In this contribution, this is taken one step forward and aC OF endowedw ith vinyl groups is used,i norder to graft sulfur to the COF skeleton through inverse vulcanization. The main aim of the article is to show the synergistic effecto fcovalent bonding and physical encapsulation of sulfur in the pores of the COF in ordert oa lleviate the fatal redox shuttling process, to improvet he cycling performance, and to provide faster ion diffusion pathways.I na ddition, it is shownh ow the materialw ith covalently-bound Sp rovides better electrochemical performance underd emanding and/or changeable charge conditions than ap arent analogue material with sulfurp hysically confined,b ut without covalent linkage.Supporting information and the ORCID identification number(s) for the author(s) of this articlecan be found under: https://doi.