Desulfurization of dimethyl disulfide (DMDS) from methyl tertbutyl ether (MTBE) has been studied on the silicalite-1/NaY core−shell composites. By changing the mass ratio of tetraethyl orthosilicate (TEOS)/ NaY, the silicalite-1 shell synthesis condition was conducted at the mass ratio of TEOS/tetrapropylammonium hydroxide (TPAOH)/ethanol (EtOH)/H 2 O = (10, 15, 20, 25, 30 g):19 g:17 g:87 g ((0.048, 0.072, 0.096, 0.12, 0.144): 0.0234:0.369:4.8293 in molar ratio, where the mass of NaY zeolite was quantified to 5 g) by a hydrothermal synthesis at 180 °C for 24 h. Results showed that when the mass ratio of TEOS/TPAOH/EtOH/H 2 O/NaY = 20 g:19 g:17 g:87 g:5 g, the silicalite-1 coating could be dispersed and covered on the surface of NaY well (the thickness of silicalite-1 shell ranged from 100 to 400 nm) with the best sulfur adsorption capacity as 20.711 mg s /g adsorbent . The shape-selective adsorption mechanism of desulfurizing DMDS from MTBE on these core−shell composites was also elaborated.