A new charge recombination layer for inverted tandem polymer solar cells is reported. A bilayer of MoOX/Al2O3:ZnO nanolaminate is shown to enable efficient charge recombination in inverted tandem cells. A polymer surface modification on the MoOX/Al2O3:ZnO nanolaminate bilayer increases the work function contrast between the two outward surfaces of the charge recombination layer, further improving the performance of tandem solar cells. An analysis of the electrical, optical, and surface properties of the charge recombination layer is presented. Inverted tandem polymer solar cells, with two photoactive layers comprising poly (3-hexylthiophene) (P3HT):indene-C60 bisadduct (IC60BA) for the bottom cell and poly[(4,8-bis-(2-ethylhexyloxy)-benzo[1,2-b:4,5-b']dithiophene)-2,6-diyl-alt-(4-(2-ethylhexanoyl)-thieno[3,4-b]thiophene))-2,6-diyl] (PBDTTT-C):[6,6]-phenyl C61 butyric acid methyl ester (PC60BM) for the top cell, yield an open-circuit voltage of 1481 mV ± 15 mV, a short-circuit current density of 7.1 mA cm−2 ± 0.1 mA cm−2, and a fill factor of 0.62 ± 0.01, resulting in a power conversion efficiency of 6.5% ± 0.1% under simulated AM 1.5G, 100 mW cm−2 illumination.