Laser ablation of Zn was performed in aqueous solution of sodium alkyl sulfate (CnH2n+1 SO4Na) with different alkyl chain lengths n. Zn nanocomposites (Zn-NC) with layered structures were obtained at specific alkyl chain lengths (n = 12, 13, 14, and 16). The interlayer spacing of Zn-NC and the tilt angle of surfactant molecules in the interlayer increased with alkyl chain length n. The increase in the tilt angle suggests the increase in packing density of surfactant molecules due to strong attraction forces between longer alkyl chains.