Microporous ETS-4 zeotype, with its 4Å pore openings, is an adequate material for the kinetic separation of nitrogen from methane. Small-sized ETS-4 was synthesized by a novel method and then utilized as membrane seeding powder. High-quality and uniform ETS-4 membranes were fabrucated utilizing a new recipe and the secondary growth approach on α-alumina supports. XRD, FESEM, and EDX studies were used to analyse the synthesized ETS-4 powder and membranes. The effect of membrane activation temperature (80-140 ºC) on permeance was evaluated. In addition to N 2 and CH 4 , the membrane permeance was also evaluated for O 2 and Ar gases. N 2 permeance increased gradually as the activation temperature was raised in the 80-120 ºC range, reaching its highest value (i.e., 2.6×10 − 8 mol m − 2 s − 1 Pa − 1 ) after activation at 140 ºC. The permeances of pure N 2 and CH 4 gases were quanti ed through the ETS-4 membrane at 30, 50, and 70 ºC, and a pressure difference up to 600 kPa. N 2 /CH 4 permselectivity of 75.19 ( N 2 permeance of 1.94 × 10 − 8 mol m-2 s − 1 Pa − 1 ) were measured at 30°C and 200 kPa of feed pressure, respectively, which is the highest N 2 /CH 4 permselectivity among all membranes reported in the literature.