The biological composite nacre, with its unique combination of stiffness, strength, and toughness has long inspired researchers to reproduce nature's achievements and synthesize structural materials using the similar design. A number of theoretical models have been developed to explain nacre's extraordinary mechanical performance, [1,2] however the exact deformation mechanisms of this material are far from being fully understood. The toughness of nacre is believed to originate from its unique micro-nanoscale ''brickand-mortar'' architecture composed of alternating layers of soft organic biopolymer and hard inorganic material (aragonite). [3][4][5][6][7] The reproduction of this highly complex structure is still beyond the current capabilities of materials processing techniques, however some morphological aspects of nacre can be imitated by a simplified nanolaminate model comprised of alternating ceramic and organic nanolayers. Several attempts to produce synthetically laminated organo-ceramic nanocomposites with nacre-like structure under ambient or biomineralization-like mild conditions have been reported. [8][9][10] These attempts mainly fall into two categories. In one, calcium carbonate or clay is used as the ceramic constituent in order to reproduce, as closely as possible, the composition and structure of nacre. [11][12][13][14][15][16] In the second category, the general design concept is to replace the relatively weak inorganic constituent found in nacre (aragonite) with structural ceramics (e.g., oxides) such as: silica, [17] alumina, [18] zinc oxide, [19] titania [20] and zirconia, [21] with the goal of producing structural composite materials with high performance. In both cases, a polyelectrolyte based layer-by-layer (LbL) technique [22] demonstrated an advantage in the preparation of simplicity, uniformity, and precise width control while preparing the organic layer. [23] Nanoindentation has been extensively used to evaluate the elastic modulus and hardness of nanolaminates. Very few reports on nanoindentation testing of man-made inorganic-organic laminates can be found in literature. Characterization by nanoindentation of other hard-soft structures such as ceramic-metal nanolaminates is more widely reported, however the results are often contradictory. For example, Wang et al. [24] found that the hardness of TiC/metal (Cr, Mo, and Fe) multilayer nanostructures synthesized by ion beam sputtering was higher than that of pure TiC. Conversely, for SiC/Al sputtered nanolaminates, reported by Chawla et al. [25] , both hardness and elastic modulus measured employing nanoindentation fell in-between the corresponding values forThe present research is motivated by the remarkable toughness of natural nanostructured composites, specifically nacre, whose highly regular ''brick-and-mortar'' structure is composed of alternating layers of aragonite sheets separated by thin layers of organic material. Robust multilayer zirconium oxide (ZrO 2 )-organic nanolaminates are deposited on Si wafers. Organic layers are synt...