A series of 2‐o‐arylidineaminophenylindoles and their cyclic derivatives (indolo[1,2‐c]quinazolines) were synthesized. The reactions occurred under relatively mild conditions and afforded the desired product in good yields. Molecular structures of the synthesized compounds were confirmed by IR, 1H‐NMR, 13C‐NMR, MS spectra, and elemental analyses. Furthermore, all the final products were screened for