Abstract: | A novel multifunctional conjugated polymer (RCP‐1) composed of an electron‐donating backbone (carbazole) and an electron‐accepting side chain (cyanoacetic acid) connected through conjugated vinylene and terthiophene has been synthesized and tested as a photosensitizer in two major molecule‐based solar cells, namely dye sensitized solar cells (DSSCs) and organic photovoltaic cells (OPVs). Promising initial results on overall power conversion efficiencies of 4.11% and 1.04% are obtained from the basic structure of DSSCs and OPVs based on RCP‐1, respectively. The well‐defined donor (D)‐acceptor (A) structure of RCP‐1 has made it possible, for the first time, to reach over 4% of power conversion efficiency in DSSCs with an organic polymer sensitizer and good operation stability. |