One of the challenges of current organic solvent nanofiltration (OSN) membranes is to improve permeability in polar and non-polar solvents without compromising selectivity. Here, the development of a new generation of OSN membranes: High flux Thin Film Composite membranes (TFC) via interfacial polymerization (IP), is proposed. This thesis offers a comprehensive study that analyses the relationship of OSN high flux TFC membrane formation and post-formation parameters, morphology, structure and surface polarity, to membrane functional performance in both polar and non polar solvents. The dissertation starts with the development of novel high flux TFC membranes for polar aprotic solvents to address the trade-off between permeability and selectivity. This is accomplished by using two different approaches: (a) incorporation of polyethylene glycol inside the pores of the support prior to the IP reaction, and; (b) post-treatment of the TFC membranes with an “activating solvent”. Subsequently, a detailed analysis of membrane performance and morphology, considering the aforementioned approaches was conducted, resulting in dramatically increased solvent fluxes without compromising rejection. Additionally, a detailed study to manipulate molecular weight cut-off (MWCO) of these TFC membranes was carried out and successfully achieved by using different amines in the IP reaction. Next, novel high flux hydrophobic TFC membranes via IP with tuned MWCO for non-polar solvents were developed, elucidated and studied. The surface properties of hydrophilic TFC OSN membranes were modified by capping the free acyl chloride groups on their surface with different monomers containing hydrophobic groups. A detailed study on surface polarity and membrane performance was undertaken, suggesting that surface chemistry plays an important role in solvent permeation. The membrane performance was compared to commercial OSN integrally skinned asymmetric (ISA) and TFC rubber-coated membranes. In the next stage of this thesis, the effects of different support membranes on TFC membrane formation and functional performance were studied for both polar and non-polar solvents. It was found that support membranes have an effect on TFC membrane formation and solvent permeation. Finally, to increase permeability even further without a requirement for treating the TFC membrane with an activating solvent, highly porous TFC membranes have been developed via IP by controlling the structure of the top layer at a molecular level. This was achieved by incorporating a monomer with a contorted structure during the IP reaction, resulting in a highly porous polymer network. It is believed high flux TFC OSN membranes prepared by interfacial polymerization may offer new degrees of freedom in membrane design, which could lead to the next generation of high performance OSN membranes.