Sluggish　redox　kinetics　and　dendrite　growth　perplex　the　fulfillment　of　efficient　electrochemistry　in　lithium-sulfur　(Li-S)　batteries.　The　complicated　sulfur　phase　transformation　and　sulfur/lithium　diversity　kinetics　necessitate　an　all-inclusive　approach　in　catalyst　design.　Herein,　a　compatible　mediator　with　nanoscale-asymmetric-size　configuration　by　integrating　Co　single　atoms　and　defective　CoTe2-x　(CoSA-CoTe2-x　@NHCF)　is　elaborately　developed　for　regulating　sulfur/lithium　electrochemistry　synchronously.　Substantial　electrochemistry　and　theoretical　analyses　reveal　that　CoTe2-x　exhibits　higher　catalytic　activity　in　long-chain　polysulfide　transformation　and　Li2S　decomposition,　while　monodispersed　Co　sites　are　more　effective　in　boosting　sulfur　reduction　kinetics　to　regulate　Li2S　deposition.　Such　cascade　catalysis　endows　CoSA-CoTe2-x　@NHCF　with　the　all-around　service　of　＂trapping-conversion-recuperation＂　for　sulfur　species　during　the　whole　redox　reaction.　Furthermore,　it　is　demonstrated　by　in　situ　transmission　electron　microscopy　that　initially　formed　electronic-conductive　Co　and　ionic-conductive　Li2Te　provide　sufficient　lithiophilic　sites　to　regulate　homogeneous　Li　plating　and　stripping　with　markedly　suppressed　dendrite　growth.　Consequently,　by　coupling　the　CoSA-CoTe2-x　@NHCF　interlayer　and　Li@CoSA-CoTe2-x　@NHCF　anode,　the　constructed　Li-S　full　batteries　deliver　superior　cycling　stability　and　rate　performance,　and　the　flexible　pouch　cell　exhibits　stable　cycling　performance　at　0.3　C.　The　gained　insights　into　the　synergistic　effect　of　asymmetric-size　structures　pave　the　way　for　the　integrated　catalyst　design　in　advanced　Li-S　systems.