Single-walled carbon nanotubes (SWNTs) have good conductivity, but their size can't match the heterojunction nanostructure in polymer solar cells (PSCs). To improve the photovoltaic performance of PSCs, herein, a faciley fabricated composite hole transport layer composed of unzipped single-walled carbon nanotubes (uSWNTs) and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is effectively applied for PSC devices. Compared with the pure PEDOT:PSS hole transport layer (HTL) without uSWNTs, the uSWNTs/PEDOT:PSS layer shows more effective performance as the hole transportation layer. Optimizing the uSWNT concentration in PEDOT:PSS results in fabrication of the PSC devices with uSWNTs/PEDOT:PSS hole transport layers that exhibit greatly improved average power conversion efficiency (PCE), from 13.72% to 14.60%, and greatly enhanced current density and fill factor, which can be ascribed to the increased conductivity and hole transport efficiency. Our approach also supports simple solution-processing techniques and the insensitivity of the performance to thickness, which promises that the faciley fabricated uSWNTs/PEDOT:PSS layer has more potential to be applicable to the roll-to-roll process of PSC fabrication with extremely low cost.