Lithium-ion batteries are a well-established technology that has seen gains in performance based on materials chemistry over the past two decades. Although there are many material selections available when assembling such a device, the fundamental design and structure remains the same - two electrodes of different potential separated by an intermediary electrolyte. Despite recent advancements with electrode materials, considerable improvements in energy density and stability are still necessary in order to achieve energy storage parity. The design of structurally oriented nanoparticles can circumvent the thermodynamic instability, undesired side reactions, high processing costs, and potential nano-toxicity effects associated with nanoparticle synthesis, processing, and use. A great deal of recent efforts have focused on the formation and understanding of ordered nanoparticle superstructures with a vast range of architectures; in particular, crystallographically oriented nanoparticle superstructures, or mesocrystals. Mesocrystals can be delineated by their high degree of crystallinity, porosity, and nanoparticle subunit alignment along a crystallographic register. Given their unique combination of nanoparticle properties and order over a microscopic size regime, mesocrystals have strong potential as active materials for lithium-ion battery electrodes. Such assemblies would possess the structural and chemical stability of microsized electrodes while exploiting the beneficial properties associated with nanosized electrodes and their large reactive surface area. (C) 2014 Elsevier Ltd. All rights reserved.