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The pharmaceutical industry has been able to tackle the emergence of new microorganisms and diseases by synthesizing new specialized drugs to counter them. Their administration must ensure that a drug is effectively encapsulated and protected until it reaches its target, and that it is released in a controlled way. Herein, the potential of layer-by-layer (LbL) structures to act as drug reservoirs is presented with an emphasis to “nano”-devices of various geometries, from planar coatings to fibers and capsules. The inherent versatile nature of this technique allows producing carriers resorting to distinct classes of materials, variable geometry and customized release profiles that fit within adequate criteria required for disease treatment or for novel applications in the tissue engineering field. The production methods of LbL reservoirs are varied and allow for different kinds of molecules to be incorporated, such as antibiotics, growth factors and biosensing substances, not limited to water-soluble molecules but including hydrophobic drugs. We will also debate the future of LbL in the pharmaceutical industry. Currently, multilayered structures are yet to be covered by the regulatory guidelines that govern the fabrication of nanotechnology products. However, as they stand now, LbL nanodevices have already shown usefulness for antifouling applications, gene therapy, nanovaccines and the formation of de novo tissues. [ABSTRACT FROM AUTHOR]