A palladium‐catalyzed tandem cyclization of 2‐(2‐ethynylphenyl)acetonitriles with isocyanides has been developed. Various indeno[2,1‐b]pyrroles were prepared in 55%–82% yields under air atmosphere at 100 °C. The key to the success of this protocol is construction of new C−C and C−N bonds via the orderly insertion of isocyanides.
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