*Address correspondence to m.shaffer@imperial.ac.uk , The bricks and mortar in the classic structure of nacre have characteristic geometry, aspect ratios and relative proportions; these key parameters can be retained whilst scaling down the absolute length scale by more than one order of magnitude. The results shed light on fundamental scaling behavior and provide new opportunities for high performance, yet ductile, lightweight nanocomposites. Reproducing the toughening mechanisms of nacre at smaller length scales allows a greater volume of interface per unit volume whilst simultaneously increasing the intrinsic properties of the inorganic constituents. Layer9by9Layer (LbL) assembly of poly (sodium 49styrene sulfonate) (PSS) polyelectrolyte and well9defined [Mg 2 Al(OH) 6 ]CO 3 .nH 2 O layered double hydroxide (LDH) platelets produces a dense, oriented, high inorganic content (~90 wt%) nanostructure resembling natural nacre, but at a shorter length scale. The smaller building blocks enable the (self9) assembly of a higher quality nanostructure than conventional mimics, leading to improved mechanical properties, approaching those of natural nacre, whilst allowing for substantial plastic deformation. Both strain hardening and crack deflection mechanisms were observed by scanning electron microscopy (SEM) during nanoindentation. The best properties emerge from an ordered nanostructure, generated using regular platelets, with narrow size dispersion.Like many natural composites, the structure of nacre, found in the inner part of some mollusk shells, is a complex hierarchical structure organized over multiple hierarchical levels leading to coupled toughening mechanisms. 196 In particular, its characteristic "brick9and9mortar" structure 7 is understood to play the key role in developing a high resistance to defects; it consists of 95 % brittle inorganic aragonite (CaCO 3 ) building blocks, around 2009900 nm thick and 59 8 Jm wide (aspect ratio from 7915), 8 "glued" together by a soft chitin9containing organic framework. This organic layer is around 209 30 nm thick 9 and makes up the remaining 5 % of the structure. The combination of a small fraction of organic phase along with this specific three9 dimensional architecture leads to exceptional mechanical properties, including high toughness (≈ 1.24 kJ.m 92 ), strength (≈ 140 MPa) and stiffness (E ≈ 60 GPa). 10,11 When loaded, the "bricks" have the ability to slide over one another within the organic phase and eventually interlock 12,13 via a range of possible mechanisms, 14 leading to strain hardening. 14,15 In addition, when a crack initiates from a defect within the nacre structure, multiple crack 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 deflections occur at the building block interfaces. 16 According to the Griffith criterion, the fracture strength of pure aragonite platelets can...