<p>The paper reports the development of ZnO-MgAl layered double hydroxides as an adsorbent-photo catalyst to remove the dye pollutants from aqueous solution and the experiments of a photocatalytic study were designed and modeled by response surface methodology (RSM) and artificial neural network (ANN). The co-precipitation and urea methods were used to synthesize the ZnO-MgAl layered double hydroxides and FT-IR, XRD and SEM analysis were done for characterization of the catalyst.The performance of the ANN model was determined and showed the efficiency of the model in comparison to the RSM method to predict the percentage of dye removal accurately with a determination coefficient (R<sup>2</sup>) of 0.968. The optimized conditions were obtained as follows: 600 <sup>o</sup>C, 120 min, 0.05 g and 20 ppm for the calcination temperature, irradiation time, catalyst amount and dye pollutant concentration, respectively. Copyright © 2016 BCREC GROUP. All rights reserved</p><p><em>Received: 22nd January 2016; Revised: 14th March 2016; Accepted:15th March 2016</em></p><p><strong>How to Cite:</strong> Hosseini, S.A., Akbari, M. (2016). ZnO/Mg-Al Layered Double Hydroxides as a Photocatalytic Bleaching of Methylene Orange - A Black Box Modeling by Artificial Neural Network. <em>Bulletin of Chemical Reaction Engineering & Catalysis</em>, 11 (3): 299-315 (doi: 10.9767/bcrec.11.3.570.299-315)</p><p><strong>Permalink/DOI:</strong> <a href="http://doi.org/10.9767/bcrec.11.3.570.299-315">http://doi.org/10.9767/bcrec.11.3.570.299-315</a></p>