Dye-sensitized solar cells (DSSCs) are low-cost photovoltaic devices that provide a high energy conversion effi ciency of 11%. [ 1 ] High conversion effi ciency, good stability, and easy fabrication are essential for commercialization of DSSCs. [ 2 ] Although DSSCs with liquid electrolytes have been reported to exhibit high effi ciency, there has been interest in developing a solid-state DSSC (ssDSSC) due to its potential to decrease the overall weight of the cells and to provide long-term durability and fl exibility. Several methods have been developed to fabricate ssDSSCs employing quasi-solid or solid polymer electrolytes. [3][4][5][6][7][8][9][10][11] In ssDSSCs, hole transporting materials (HTMs) and the control of interfacial properties between the nanoporous TiO 2 layer and the HTM are critical to the photoconversion effi ciency of the cells. Recently, HTMs have been extensively investigated as potential replacements for conventional I 3 − /I − redox electrolyte systems using iodine (I 2 ) in DSSCs. [12][13][14][15][16][17][18] As an organic HTM, spiro-OMeTAD was used for an iodine free ssDSSC and showed higher effi ciency of 5.1%. [ 17 , 18 ] Inorganic HTMs such as CuI showed a good effi ciency of 4.7%, [ 12 ] but the crystal formation of metal oxide gradually reduced cell performance. [ 19 ] Another possibility is the utilization of p-type conducting polymers, e.g., polypyrrole, polyaniline, polydiacetylene, poly (3-octylthiopehene), and poly(3,4-ethylenedioxythiophene) (PEDOT). [20][21][22][23][24][25][26] These polymers are advantageous over other small molecules due to their low cost, good stability, simple fabrication using spin-coating, and easy preparation of designable structures. Recently, Ho et al. reported an iodine (I 2 )-free ssDSSC using polyaniline/carbon black composite with imidazolium iodide derivatives, which effectively generates I − / I 3 − redox couples without addition of iodine (I 2 ). [ 27 ] However, while conductive polymers offer many advantages, they show low energy conversion effi ciencies due to poor penetration into the nanopores of TiO 2 photoelectrodes that arises from mismatches between the molecular sizes of the polymers and the pore sizes of the TiO 2 layer. Recently, Yanagida et al. were successful at improving the power conversion effi ciency signifi cantly up to 2.85%, which was the highest effi ciency for an iodine-free ssDSSC using a conductive polymer as HTM. [28][29][30] The penetration of a conductive polymer into TiO 2 porous layers was successfully improved via the in situ photoelectrochemical polymerization of a heterocyclic monomer, e.g., 2,2'-bis(3,4-ethylenedioxythiophene) (bis-EDOT). [ 29 ] However, the maximum penetration depth of the conductive polymer into the TiO 2 layer was 4-5 μ m, above which cell effi ciency was decreased, resulting from insuffi cient interfacial properties of electrode/HTM despite increased dye adsorption. More recently, Liu et al. further improved cell efficiency up to 6.1% using indoline D149 dye as a sensitizer, [ 31 ] whe...