AbstractA facile electrophoretic deposition method was successfully applied to achieve novel nanoclay-reinforced polyacrylamide nanocomposite thin films. A special curled architecture of the re-aggregated nanoclay-platelets was identified, providing a possible source for realizing the interlocking mechanism in the nanocomposites. The curled architecture could be the result from strain releasing when the thin films were peeled off from the substrates. Through micro-/nano-indentation and in situ observation of the deformation during tensile test with an atomic force microscope (AFM), the localized deformation mechanism of the synthesized materials was investigated in further details. The results implied that a localized crack diversion mechanism worked in the synthesized nanocomposite thin films, which resembled its nature counterpart-nacre. The deformation behavior and fracture mechanism were discussed with reference to lamellar structure, interfacial strength between the nanoclays and the polyacrylamide matrix, and nanoclay agglomeration.