Two-component suspensions of titania and halloysite nanotubes (HNTs) were prepared in ethanol with 0.5g/L (optimum concentration) of polyethyleneimine (PEI) and different wt% of HNTs. Kinetics of Electrophoretic deposition (EPD) decreased with increasing the HNTs content in suspensions due to their less mobility compared with titania particles. HNTs reinforced the microstructure of coatings and reduced or completely prevented from cracking during drying and heat-treatment steps. Removal of methylene blue (MB) via adsorption by HNTs coatings was faster than its photocatalytic degradation by titania coating. Dispersion of HNTs (up to approximate to 30wt%) in the matrix of titania resulted in the synergistic catalytic effect in MB removal. The synergistic effect was because of the shorter traveling distance of MB molecules adsorbed on HNTs toward the photocatalytic active site of titania particles in composite coatings. However, the synergistic effect was destroyed with increasing the HNTs content in coating. Difference between the amount of MB removed by titania and composite coatings increased at longer times (60minutes). Mass transfer of MB adsorbed on HNTs toward the photocatalytic active sites of adjacent titania particles can compensate the decline in the mass transfer from solution at longer times.