Abstract: The electronic structure and chemical bonding of Sm(Ind)₃ have been studied by INDOcalculation. The results show that the 6s, 6p and 5d orbitals of Sm are mixed with the atomic orbitals of ligands to some extent while the 4f orbitals of Sm are strongly localized, participating in bonding less than 2%. The HOMOand the LUMOare of π-type. The chemical bonds of Sm(Ind)₃ are considerably covalent in character. The net charge distribution on the carbon atoms of the indenyl group is unequal. Based on packing of ligands the possibility of existence of Sm-C σ bonds in Sm(Ind)₃·THFwas discussed.