papers have shown that converting bulk powder to 2D nanosheets yields significant capacity increases. [18][19][20] In addition, 2D platelet-shaped nanoparticles show great potential for use in battery electrodes due to shorter solid state diffusion lengths which can yield improved rate performance. [21] However, high aspect ratio 2D nanosheets can reduce the diffusion coefficient associated with ion transport within the electrolyte filled pores. [21] To avoid slow liquid phase diffusion while maintaining short solid state diffusion times, quasi-2D platelets with reduced aspect ratio are required. [21] This suggests that when using Fe 2 O 3 for battery applications there would be significant advantages to producing it in the form of quasi-2D platelets.Several synthetic routes have been proposed to generate nanoscale α-Fe 2 O 3 of various geometries including 2D platelets. [22][23][24][25] However, current methods are expensive to implement and typically include multiple complex steps which require high temperatures as well as templates or solid supports. A simpler alternative is to use a controllable, soft interfacial method to self-assemble well-defined and mesoporous nanostructures at an immiscible aqueous/organic interface. [26] The interface provides a defect-free, dimensionally-confined space to self-assemble unique 2D nanomaterials in a single step with perfect reproducibility. This can yield nanomaterials, potentially including quasi-2D materials, that are inaccessible in bulk solution. [27,28] Furthermore, certain interfaces between two immiscible electrolyte solutions (ITIES) may be electrochemically polarized, providing a driving force that may influence the kinetics of self-assembly or even enable electrosynthesis of interfacial thin films of materials. [29,30] Another consideration involves electrode architecture and the need to include conductive additives. For Fe 2 O 3 , a number of carbon-based additives including 2D graphene, 1D carbon (nanofibers/nanotubes), and 0D nanocarbon has been extensively explored. [10,[31][32][33][34] We believe significant advantages are to be had from using carbon nanotubes (CNTs) as the conductive additive. We and others have shown that incorporating CNTs in electrodes based on both 2D [35][36][37] and 3D [38] materials allows them to approach their theoretical capacity. This is because the high conductivity of the CNTs allows effective charge distribution increasing both initial capacity, stability, and rate performance. [38][39][40] In addition, CNTs provide mechanical reinforcement to the electrode without the need for any additional binder. [38] This is particularly important for iron oxide-based anodes, where a large volume expansion is often observed upon lithiation which leads to particle de-cohesion and poor cycling performance. [7] We have shown previously that nanotubes lead to electrode toughening which imparts stability even in silicon anodes which display very high volume expansion. [38] In this paper we will combine the advantages associated with quasi-2D...