Nanocomposites are the emerging materials of the 21st century in view of their possessing design uniqueness without any compromises, certain unusual property combinations that are not found in conventional composites, as well as a wide spectrum of applications. Polymer-based layered compound nanocomposites have special place in view of their best property enhancement. Hence, the objective of this article is to bring new ideas to optimize the design of polymer/layered compounds/fibrous nanocomposites, starting with a brief overview of the preparation, structure, properties and applications. The proposed strategy suggests the use of synthetic and natural layered compounds, taking into account their ability to be exfoliated in the form of single layers, which can be chemically grafted with key molecules. The same procedure can also be applied to fibrous materials. These surface-grafted molecules can carry reactive groups to be bonded to the polymer matrices. Thus adhesion between the reinforcement and the polymer matrix can be achieved. This methodology, which has not been explored systematically in the specialized literature, can be used to produce polymer nanocomposites with low-cost fibrous materials having similarity to expensive carbon nanotubes exhibiting optimized dispersion, interfacial bonding, and attractive physical and other properties.