A new class of dithiosquarylium dyes (DTSQ) has been synthesized by the reaction of squarylium dye (SQ) with Lawesson's reagent or P 4 S 1 0 . The λ m a x , of DTSQ dyes undergoes a bathochromic shift of about 25 nm compared with corresponding SQ dyes. The visible absorption spectra of DTSQ dyes are well accounted for by Pariser-Parr-Pople Molecular Orbital (PPP-MO) calculations. Electrophotographic characteristics of negatively charged dual layered photoreceptors with DTSQ for charge generation materials (CGM) and 1-phenyl-1,2,3,4-tetrahydroquinoline-6-carboxyaldehyde-1',1'-diphenylhydrazo ne as a charge transport material (CTM) have been investigated. The photoreceptor that used DTSQs exhibited high photosensitivity at white light.