Recently, layered double hydroxides (LDHs) have gathered vast interest due to overall positive charge, unique crystallinity, and biocompatibility for diverse applications. Despite the advantageous attributes, these hydrotalcites often result in several limitations concerning the application requirements, such as aggregation, as well as poor chemical and thermal stabilities, hindering their scale‐up progress and practical utilization. In addressing these issues, the recent advancements in the fabrication of intelligent LDHs nanocomposites based on organically (polymer/polyelectrolyte)‐modified and inorganic (metal)‐composited architectures are systematically presented. Initially, a brief note on the shortcomings in various fields and the chemistry of these pristine LDHs is given. Then, various synthetic strategies used to fabricate these emerging LDH nanocomposites are comprehensively emphasized, focusing on the advancements in their structure and applicability. In addition, the effects of various attractive physicochemical attributes of LDHs and their nanocomposite forms are discussed, including their applicability in adsorption, biomedicine, catalysis, energy, and environment‐related applications. In summary, this article is concluded with an outlook concerning the positioning of LDH‐based nanocomposites compared to other innovative materials, as well as the current challenges and future requirements for scale‐up.