Silicalite-1 monolayers on alpha-Al2O3 supported polymer thin films with strong zeolite-polymer bonding, high surface coverage, uniform orientation in b-axis, and easy control of assembly could be manufactured by the stacking and sonication assembly or by the simpler manual assembly (see the figure). The methodology can be further applied to the monolayer assembly of various nano- and micro-sized particles with surface hydroxyl groups to porous solid supported polymer thin films.