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Here, we synthesized metal-free organic dye (CCPICPB) with two carbazole donor groups and two anchoring groups that exhibit a panchromatic absorption in the near-infrared range of up to 750 nm. To study the photophysical properties of synthesized CCPICPB dye, the UV–Vis and cyclic voltammetric experiments were studied and the obtained results were validated with theoretical simulation studies. After that, the solvothermal approach is used to synthesize pristine anatase and calcium (Ca)-doped TiO2 microspheres with a smooth morphology. These microstructures are examined in depth using XRD, electron microscopy and electrochemical analysis methods. On TiO2 and Ca-doped TiO2 photoanode materials, we first evaluated the performance of CCPICPB dye. Upon our optimized experimental condition, the 3% Ca-TiO2 photoanode-based device exhibits an efficiency of 4.04%, which is greater than that of the pristine TiO2 photoanode-based device (2.93%). Because of the quicker electron transport in the Ca-TiO2 film, the short-circuit current density and efficiency of DSSCs were improved. Moreover, when the CCPICPB dye was used as a co-sensitizer with the common Ru(II) dye (Z907), interestingly it showed the highest efficiency (6.11%) when compared with Z907 alone (5.12%). This improved efficiency of the co-sensitized device resulted from greater VOC conjugated with improved JSC. The JSC was improved because CCPICB dye could compensate for the photocurrent loss caused by redox electrolyte while the VOC was improved because electron recombination was inhibited under the co-sensitization conditions. [ABSTRACT FROM AUTHOR]