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The coordination states of the divalent and trivalent rare earth complexes in ionic liquid, triethyl-pentylphosphonium bis(trifluoromethyl-sulfonyl) amide [P2225][TFSA] were investigated by Raman spectroscopy and DFT calculation. The concentration dependences of the deconvoluted Raman spectra were investigated for 0.23-0.45 mol kg-1 RE(III), RE=Nd and Dy, and the mixed sample of RE(II)/RE(III)=1/3 at the molar ratio in [P2225][TFSA]. According to the conventional analysis, the solvation number; n of rare earth complexes in [P2225][TFSA] were determined to be n=4.06 for Nd(II), 5.01 for Nd(III), 4.12 for Dy(II) and 5.00 for Dy(III).-1 , respectively. This result was revealed that [RE (III) (cis-TFSA)5] 2cluster formed stronger coordination bonds than [Dy (II) (cis-TFSA)4] 2cluster. The average atomic charges and the bond distances of these clusters were consistent with the thermodynamic properties.