Compounds having imidazo[5, 1‐a]isoquinoline nucleus have been synthesised. Selenium dioxide oxidation of a mixture of various aldehydes and 1‐isoquinolinemethylamine yielded the respective 3‐substituted imidazo[5, 1‐a]isoquinolines in good yields. When 1‐isoquinolinemethylamine was employed without any aldehyde, 3‐(1‐isoquinolinyl)imidazo[5, 1‐a]isoquinoline (IQ‐1) was isolated. This IQ‐1 is fluorescent and all the compounds were thoroughly characterized. Molecular structures of IQ‐1 and 3‐(2‐hydroxyphenyl)imidazo[5, 1‐a]isoquinoline (IQ‐4) have been confirmed by single crystal X‐ray diffraction technique.
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