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The oligomerization of phenyl isocyanate catalyzed by divalent bis(methylcyclopentadienyl)samarium complex was studied. The initiating reaction and the effect of coordination environment around the samarium atom were mainly discussed. It is found that the initiation reaction has a great influence on the apparent catalytic activity. The oligomers can be split into two fractions. The methanol insoluble fraction is mainly composed of dimers, while the methanol soluble fraction is mainly composed of trimers. Neither SmI2 nor SmI2(hmpa)4 (hmpa＝hexamethylphosphoric triamide) shows catalytic activity for the oligomerization of phenyl isocyanate.