The effect of Eu3＋ ion doping in the La sites of single-crystal La4/3Srs/3Mn2O7 was investigated. Electron spin resonance （ESR） was applied to La4/3Sr5/3Mn2O7 and （Lao.8Euo.2）4/3Sr5/3Mn2O7 single crystals. A phase separation and phase transitions were observed from the ESR spectra data. Between 350 K and 300 K, both paramagnetic resonance （PMR） and anisotropic ferromagnetic resonance （FMR） lines were observed in the ab plane and the c axis direction, suggesting a coexistence of the paramagnetic （PM） phase and the ferromagnetic （FM） phase. The magnetization measurement reveals a spin-glass-like behavior in single-crystal （Lao.8Euo.2）4/3 Sr5/3Mn2O7 below the temperature of spin freezing Tf （- 29.5 K）.
