This paper presents data for the synthesis and characterization of layer double hydroxides (LDH) and their use for color and chemical oxygen demand (COD) removal from effluents generated by a textile industry. Adsorption studies with raw and biologically treated (activated sludge) textile effluent showed that the pseudo-second order model best fitted the experimental data, leading to adsorption coefficients of 39.1 and 102.9 mgCOD/gLDH for raw and treated effluents, respectively. The best conditions for color and COD removal were obtained at lower values of temperature and pH (25 °C and pH 7) and, in these conditions, an LDH dose of 10 g/L resulted in color removal efficiencies of 56% for samples of raw and 66% for samples of treated effluent. Recycling studies indicated that the reuse of thermally treated LDH led to a progressive loss in the removal efficiencies of COD and color. The reduction was more pronounced with samples of the raw textile effluent. LDH characterization performed before and after each adsorption and regeneration experiment showed that there was no intercalation of dye molecules in the interlayer region of the LDH, indicating that COD and color removal might be due to the adsorption of organic molecules onto the LDH surface.