Please cite this article as: Khan, U., May, P., O'Neill, A., Coleman, J.N., Development of stiff, strong, yet tough composites by the addition of solvent exfoliated graphene to polyurethane, Carbon (2010), doi: 10.1016/j.carbon. 2010.07.008 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.Development of stiff, strong, yet tough composites by the addition of solvent We have prepared graphene dispersions, stabilised by polyurethane in tetrahydrofuran and dimethylformamide. These dispersions can be drop-cast to produce free-standing composite films. The graphene mass fraction is determined by the concentration of dispersed graphene and can be controllably varied from 0% to 90%. Raman spectroscopy and Helium ion microscopy show the graphene to well-dispersed and well-exfoliated in the composites, even at mass fractions of 55%. On addition of graphene, the Young's modulus and stress at 3% strain increase by ×100, saturating at 1 GPa and 25 MPa respectively for mass fractions above 50wt%. While the ultimate tensile strength does not vary significantly with graphene content, the strain at break and toughness degrade heavily on graphene addition. Both these properties fall by ×1000 as the graphene content is increased to 90wt%. However, the rate of increase of Young's modulus and stress at 3% strain with mass fraction is greater than the rate of decrease of ductility and toughness.This makes it possible to prepare composites with high modulus, stress at low strain and ultimate tensile strength as well as relatively high toughness and ductility. This could lead to new materials that are stiff, strong and tough. With this in mind, we propose a different approach. Rather than reinforcing thermoplastics, we suggest that graphene might make an impact reinforcing elastomers.Reinforcement mechanisms in elastomeric composites are more complex than in thermoplastic based composites, a fact that may circumvent the poor stress transfer described above. Hard thermoplastics are characterised by relatively high stiffness and strength but low ductility and toughness (work done to fracture). Conversely, elastomers are characterised by low stiffness and low stress at low strain but high ductility and toughness. We propose that addition of graphene to elastomers could result in a material with positive elements of both hard thermoplastics and elastomers: high stiffness and strength yet relatively large ductility and toughness. Such materials would be useful in a range of applications.For such composites to have the properties outlined, a delicate balance must be maintained. While addition of nano-fillers such as nanotubes, nano...