It is found that the breaking-bond at the crystal edge of halloysite nanotubes and chrysotile nanotubes have different proton adsorption capacity due to the difference of electronegativity between Al3+ and Mg2+ in the crystal structure, so they carry negative and positive charges respectively in near-neutral solution, which leads to the adsorption capacity of ChNTs with positive charges to MO is greater than that of HNTs.