We demonstrate that nanocrystalline Al-doped zinc oxide (n-AZO) thin film used as an electron-extraction layer can significantly enhance the performance of inverted polymer solar cells based on the bulk heterojunction of poly[[9-(1-octylnonyl)-9H-carbazole-2,7-diyl]-2,5-thiophenediyl-2,1,3-benzothiadiazole-4,7-diyl-2,5-thiophenediyl] (PCDTBT) and [6,6]-phenyl C71-butyric acid methyl ester (PC70BM). A synergistic study with both simulation and experiment on n-AZO was carried out to offer a rational guidance for the efficiency improvement. As a result, An n-AZO film with an average grain size of 13 to 22 nm was prepared by a sol-gel spin-coating method, and a minimum resistivity of 2.1 × 10-3 Ωcm was obtained for an Al-doping concentration of 5.83 at.%. When an n-AZO film with a 5.83 at.% Al concentration was inserted between the ITO electrode and the active layer (PCDTBT:PC70BM), the power conversion efficiency increased from 3.7 to 5.6%.