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The structural orientation of an amphiphilic crystalline polymer to ah ighly ordered microphase-separated lamellar structure on ah ydrophobic surface is presented. It is formed by the surface graft polymerization of poly(ethylene glycol)behenyl ether methacrylate onto poly(trimethylsilyl) propyne in the presence of allylamine.Inparticular,allylamine playsapivotal role in controlling the crystalline phase, configuration, and permeation properties.T he resulting materials are effectively used to improve the CO 2 capture property of membranes.U pon the optimization of the reaction conditions,ahigh CO 2 permeability of 501 Barrer and aC O 2 /N 2 ideal selectivity of 77.2 are obtained, whichexceed the Robeson upper bound limit. It is inspiring to surpass the upper bound limit via as imple surface modification method. Scheme 1. Free-radical graft polymerization of PEGBEM onto PTMSP.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.