The IR absorption spectra of “cation cation” coordination compounds for Np(Ⅴ) U(Ⅵ) has been studied in HNO 3 and HClO 4 solution. By investigating the influence of ions concentration and acidity on spectrum, the coordination compound behavior between Np(Ⅴ) and U(Ⅵ) is explained at various conditions. Meanwhile, the possible mechanism of coordination compound is represented.