In spite of significant interest in 2D nanofillers, the effect of polymer intercalation on properties remains poorly understood. We use automated spray deposition to form two families of well-aligned polymer/clay nanolaminates that differ by one methyl group in the clay modifier; this difference results in intercalation in one instance and no intercalation in the other. Dynamic mechanical properties and gas permeability are reported alongside micromechanical and barrier models and a detailed description of the structures and phases present. Observed variations in modulus cannot be explained by micromechanical models often applied to polymer nanocomposites. In contrast with "effective particle" arguments, barrier properties are dominated by single layer aspect ratios. These findings have relevance for all manner of "bricks and mortar" hybrids. Additionally, these systems represent the macroscopic equivalent of the multilayer stacks found in practically all nanocomposites, with wide-ranging implications for nanocomposite design and properties more generally.