Surface modified Mg-Fe layered double hydroxide materials by CTAB are used for photo catalytic degradation of methyl orange. Mg-Fe LDH (material-1) was prepared by co-precipitation method and material-2 was prepared by intercalation of CTAB into material-1. Further, calcination and surface modification of material-2 was done to get material-3.All these materials were characterized by FT-IR. Structure and composition was confirmed by XRD and SEM with EDX. Surface area of prepared material 1,2 and 3 was determined by BET analysis and the values of surface area are 28.54, 18.29 and 4.95m2 /g and pore size is 10.6, 7.9 and 9.2 nm respectively. The band gap values obtained on the basis of DRS studies for materials-1,2 and 3 are 3.9 , 3.9 & 3.2 eV respectively. Photo catalytic degradation of methyl orange using material 1, 2 & 3 in the presence of 10 W LED bulb was studied under identical conditions and progress of the reaction was monitored by UV-Vis spectrometer. The catalytic efficiency of material 3, 2 and 1 is 90%, 32%, 2% respectively. Decreasing in particle size after surface modification and enhanced mesoporous nature accounts for the highest catalytic efficiency of material -3 and it is cost effective easy to prepared and eco-friendly.