mesoporous charge transfer layer, their application into the fl exible electronics would be limited due to their brittleness and the high-temperature (i.e., T > 450 °C) sintering process which damages plastic substrates. Otherwise, solutionprocessed planar heterojunction (SP-PHJ) PrSCs can be fabricated using low-temperature processable interlayers without mesoporous metal oxides; this approach enables the fabrication of fl exible PrSCs on plastic substrates. [7][8][9] Therefore, the development of a solution-processed and effi ciently charge-transporting interlayer material has been required recently to increase PCE of SP-PHJ PrSCs for the practical application of highly effi cient and fl exible PrSCs. In addition to conducting polymers (e.g., poly(3,4-ethylen edioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), [ 7,9,15,16 ] self-organized hole extraction layer (SOHEL) [ 9 ] ), several different hole transport materials (HTMs), including inorganic materials (graphene oxide, [ 17 ] reduced graphene oxide, [ 18 ] NiO x [ 15 ] ) and conjugated polymers (e.g., PolyTPD, [ 19 ] P3HT, [ 20 ] poly(2,5-(2-octyldodecyl)-3,6-diketopyrrolopyrrole-alt-5,5-(2′,5′di(thien-2-yl)thieno[3,2-b]thiophene) (DPP-DTT), [ 21 ] PCP-DTBT, [ 21 ] and PCDTBT [ 21 ] ) have been used to increase the PCE in SP-PHJ PrSCs.Among these materials, polymeric HTMs have been intensively developed for highly effi cient SP-PHJ PrSCs because they can be fabricated by solution processing and exhibit better hole mobility compared to vacuum-processed small-molecule HTMs. [ 3 ] In the fi rst few papers reporting SP-PHJ PrSCs, they were based on the PEDOT:PSS HTM [ 16 ] because PEDOT:PSS is one of the most commonly used HTMs for organic photovoltaics [22][23][24][25][26][27] and organic light-emitting diodes (OLEDs). [ 28,29 ] However, work function (WF) of PEDOT:PSS (≈4.9-5.2 eV) is highly dependent on the ratio of the polymeric acid, PSS relative to PEDOT [ 25,28 ] and therefore may not be suffi ciently high to perfectly match the valence band maxima (VBM) of perovskite materials (e.g., -5.43 eV for methylammonium lead iodide (MAPbI 3 )) for ohmic contact and consequential effi cient charge extraction. [ 9,15,[19][20][21][22][23][24][25][26][27][28][29] Moreover, PEDOT:PSS is dispersed with a large particle size (≈60 nm) in solution; [ 30 ] it precipitates slowly from the solution during storage and is diffi cult to redisperse from the aggregated Organic-inorganic hybrid perovskite solar cells are fabricated using a watersoluble, self-doped conducting polyaniline graft copolymer based on poly(4styrenesulfonate)-g -polyaniline (PSS -g-PANI) as an effi cient hole-extraction layer (HEL) because of its advantages, including low-temperature solution processability, high transmittance, and a low energy barrier with perovskite photoactive layers. Compared with conventional poly(3,4-ethylenedioxythiop hene):poly(styrene sulfonate) (PEDOT:PSS) dispersed in water solution, PSSg-PANI molecules are dissolved in water because of the polymeric dopant covalently bonde...