Aim To study the influences of pH values in solusion and anionic L-(L-=Cl-,NO-3) to the crystal growing of [ Ni(II)(Dipha)(Benzidine) ] under hydrothermal conditions.Methods The hydrothermal method is used to synthesize [ Ni(II)(Dipha)(Benzidine) ] and prepare its crystal.Results The experimental results shown that optimum conditions of the crystal growing are pH≈7.0,Ni salts are either NiCl2 or Ni(NO3)2 to easily produce coordination crystal,A series crystals were synthesized by the hydrothermal method.Conclusion In this system,[ Ni(II)(Dipha)(Benzidine) ],pH≈7 and a appropriate L-are all necessary conditions for crystal formation and growth.