Myristic, hexanoic, and succinic acids were incorporated into a lithiumand aluminum-containing layered double-metal hydroxide (LDH), resulting in materials with interlayer spacings of 21.6, 17.8, and 7.5 A, respectively. Comparison of these spacings with the dimensions of the all-trans form of the acid molecules indicates an interlayer monolayer arrangement for myristic and succinic acids, and a bilayer arrangement for hexanoic acid. Sorption isotherms of pyrene by these organic-exchange LDH's were carried out in methanol/water mixtures, because of the limited solubility of pyrene in water. Using cosolvent theory, partition coefficients (log KM) for pyrene into myristic acid-LiAl-LDH and hexanoic acid-LiAl-LDH were determined to be 4.38 and 3.44, respectively. No sorption of pyrene was observed in succinic acid-LiAl-LDH, suggesting that partitioning into the interlayer space was controlled by the width of the interlayer spacings. Infrared studies showed distortion of the acid chain packing upon incorporation of pyrene into hexanoic acid-LiAl-LDH. The conclusions of this study are that organic-exchanged LDH's exhibit novel sieving effects toward hydrophobic compounds based on interlayer spacings, and that the interlayer packing of the alkyl chains influences the extent of sorption.