Display omitted •The LDHs and LDO were prepared and characterized to catalyze removal nitrogen element in hydrochar.•Mg-Al LDO showed the highest efficiency for the removal of nitrogen among the catalysts.•Partial floc directly transformed to hydrochar according to “solid-solid” reaction.•The possibility reaction pathways of removal nitrogen during HTC were proposed. The high content of nitrogen in hydrochar produced from hydrothermal carbonization (HTC) of sewage sludge (SS) leads to serious NOx pollution when the hydrochar is used as a solid fuel. Mg-Ga layered double hydroxides (LDHs), Mg-Al LDHs and their calcined samples (layered double oxides, LDO) were prepared. The LDHs and LDO all can notably promote the removal of nitrogen element, in which organic-N was transferred to NH4+-N to cause increasing pH value. Mg-Al LDO showed the highest efficiency for the removal of nitrogen among the catalysts. The thermal decomposition of the N-organic matter with acidic sites in catalyst was the key step to release NH3. The key role of basic sites in Mg-Al LDO was that it can effectively destroy the cell wall and extracellular polymeric substances structure. The lipid-like substance did not participate in the carbonization reaction, but they can be absorbed by the hydrochar. Partial SS floc directly transformed to hydrochar according to “solid-solid” reaction. The reaction pathways of remove nitrogen were proposed.