Through deposition of APTES-functionalized Al2O3 particles onto a coarse macroporous support, a new strategy to reduce the pore size and simutaneously promote a high density of heterogeneous nucleation sites was developed, and a continuous and thin ZIF-8 membrane exhibiting remarkably high H2 permeance of 5.73 × 10(-5) mol m(-2) s(-1) Pa(-1) and H2/N2 ideal selectivity of 15.4 was achieved.