Angle-resolved photoemission spectra have been measured to study the electronic structures of Ni intercalated layered compound Ni1/3TiS2. The results have shown that some new bands appear in Ni1/3TiS2 and the dispersions of most other bands are strongly modified compared with TiS2. It is clarified that the new band near the Fermi level (EF) is the split-off state or the bonding state between the final states originating from the |d1(t2g)〉 and |d2(t2g,eg)L〉 initial states, where L stands for the S 3p hole state. Another new band observed at ∼1 eV below EF is hardly dispersive and attributed to the Ni 3dz2-Ti 3dz2 bonding state. The Ni 3d"eg"-S 3p bonding states are observed in the larger binding energy region. Knowledge of hybridizations among the 3d states of the intercalant, Ti 3d states, and S 3p states are essential to interpret the physical properties of Ni1/3TiS2.