ABSTRACTMg-, Al and Mg-, Cu-, Al-layered double hydroxides well-known synthetic hydrotalcite-like sorbents, were used for the first time as carriers for indicators in the sorption catalytic determination of copper(II) and L-α-alanine. Mg-, Al and Mg-, Cu-, Al-layered double hydroxides were synthesized by coprecipitation and characterized using infrared spectroscopy, X-ray diffraction, and scanning electron microscopy. The adsorption of 0.50 mg L−1 copper(II) solution by Mg-, Al-layered double hydroxides followed a pseudo-second-order model with an equilibrium sorption capacity of 24.2 × 10−3 mg g−1 (3.8 × 10−4 mmol g−1) and a reaction rate constant of 4.2 g mg−1 min−1. Mg-, Al-layered double hydroxide tablets were prepared and used for sorption concentration and subsequent sensitive and selective sorption catalytic determination of 5.5 × 10−3 to 1.0 mg L−1 copper(II) at the sorbent phase. The method was used for the analysis of natural water. A method was developed for the determination of α-alanine in Mg-, Cu-, Al-layered double hydroxide tablets with a limit of detection of 4.0 × 10−3 mol L−1. In addition, thin layers of Mg-, Cu-, Al-layered double hydroxide were used to separate α-alanine and determine α-amino acids by thin-layer chromatography.