The four-cyclic condensed aromatic ketone 7H-benz[de]anthracene-7-one and its derivatives belong to the class of important anthraquinoid dyes, including laser and luminescent dyes. Current work is devoted to the synthesis of 3-cyanobenzanthrone and its evaluation of being a useful precursor for obtaining new 3-substituted derivatives with heterocyclic moieties, a handful of which have been synthesized up to now. The photophysical properties of the prepared compounds are investigated. The synthesized derivatives have pronounced fluorescence and are fluorescent “turn-off” probes for acidic environment. Therefore, these compounds can be used for pH sensing and as dyes in materials science and for visualization of biological structures.