Green synthesis of nanosized AlPO-n and SAPO-n (n = 5 and 18) crystals with AFI and AEI type structures from non-reacted precursor suspensions with an essential chemical compensation is presented. The crystallization of both materials was accomplished within few minutes (5-18 minutes) instead of several days by replacing the conventional with microwave heating. The nanosized AlPO-n and SAPO-n (n = 5 and 18) crystals were stabilized in coating suspensions and deposited in layers on silicon wafers. It is shown that the AFI-type crystals (one-dimensional pores with a diameter of 0.73 nm) were primarily oriented with (001) direction perpendicular to the substrate, while the AEI-type crystals (three-dimensional pores with a diameter of 0.38 nm) were randomly oriented. The relationship between the crystal orientation and the adsorption behavior of the AFI and AEI layers toward water was studied by GI-XRD and operando IR spectroscopy.