This paper reports the application of anthracite particles of different sizes and coated with nine kinds of layered double hydroxides (LDHs) varying in M(II)-M(III) cations, as alternative substrates in the simulated vertical-flow constructed wetland columns. Effects of LDHs-coating and particle size of modified anthracites were examined to evaluate their abilities in removing oxygen demand and nitrogen from sewage wastewater. Results showed that LDHs modification effectively enhanced the removal of nitrogen and organics. The removal efficiencies of total nitrogen (TN) , ammonia and chemical oxygen demand (COD) were best improved by 28.5%, 11.9% and 4.1% for the medium particle size (1-3 mm), followed by 9.2%, 5.5% and 13.6% for the large size (3-5 mm), respectively. Only TN removal was improved up to 16.6% for the small particle size (0.5-1 mm). Nitrate tended to accumulate and fluctuate greatly across all the treatments, probably due to the dominancy of aerobic condition in the vertical-flow columns. Overall, MgFe-LDHs was selected as the best-modified coating for anthracite. The results suggested LDHs modification would be one of the promising strategies to provide new-types of highly efficient and lasting wetland substrates.