Layered double hydroxides (LDHs) have attracted considerable attention as promising materials for electrochemical and optical sensors owing to their excellent catalytic properties, facile synthesis strategies, highly tunable morphology, and versatile hosting ability. LDH-based electrochemical sensors are affordable alternatives to traditional precious-metal-based sensors, as LDHs can be synthesized from abundant inorganic precursors. LDH-modified probes can directly catalyze or host catalytic compounds that facilitate analyte redox reactions, detected as changes in the probeâs current, voltage, or resistance. The porous and lamellar structure of LDHs allows rapid analyte diffusion and abundant active sites for enhanced sensor sensitivity. LDHs can be composed of conductive materials such as reduced graphene oxide (rGO) or metal nanoparticles for improved catalytic activity and analyte selectivity. As optical sensors, LDHs provide a spacious, stable structure for synergistic guestâhost interactions. LDHs can immobilize fluorophores, chemiluminescence reactants, and other spectroscopically active materials to reduce the aggregation and dissolution of the embedded sensor molecules, yielding enhanced optical responses and increased probe reusability. This review discusses standard LDH synthesis methods and overviews the different electrochemical and optical analysis techniques. Furthermore, the designs and modifications of exemplary LDHs and LDH composite materials are analyzed, focusing on the analytical performance of LDH-based sensors for key biomarkers and pollutants, including glucose, dopamine (DA), H2O2, metal ions, nitrogen-based toxins, and other organic compounds.