having broader absorption ranges, which span a larger portion of the solar spectrum. [ 5,6 ] Nevertheless, organic semiconductors used in PSCs having a single BHJ layer still present narrow absorption ranges that cover only a fraction of the solar spectrum; leaving more than 60% of the total photons unabsorbed. [ 7 ] Furthermore, the maximum thickness of this BHJ layer allowable for high effi ciency is limited by the transit-time of carriers within this layer. For a given set of materials and processing conditions, the optimum BHJ layer thickness strikes the best compromise between maximizing photon absorption and charge collection. [ 8 ] To overcome the limitations of PSCs with a single BHJ layer, two or more PSCs having BHJ active layers with complementary absorption ranges are connected in series by stacking them on top of one another. These so-called tandem solar cells can achieve higher power conversion effi ciency (PCE) values than single BHJ layer PSCs because they cumulatively absorb a larger portion of the solar spectrum. When the sub-cells are connected in series in a tandem PSC, the open-circuit voltage ( V OC ) of the sub-cells ideally adds up while the short-circuit current density ( J SC ) is limited by the smallest J SC generated in any of the sub-cells. [ 7,[9][10][11][12] A critical component to produce effi cient tandem PSCs is the charge recombination layer (CRL) that connects the two adjacent sub-cells. The CRL that is sandwiched between the sub-cells, needs to allow holes to be collected from one sub-cell and recombine with the electrons collected from the other sub-cell, while allowing photons to pass through it and illuminate the adjacent sub-cell. Furthermore, the CRL should have low electrical resistance to minimize power density losses. Therefore, materials comprising the CRL are required to have low absorption in the spectral region of interest, be suffi ciently conductive, and provide a large work function (WF) contrast between the two outward surfaces in contact with the photoactive layers. In addition, in tandem PSCs, the CRL also needs to allow for the fabrication of a solution-processed top photoactive layer. [ 7 ] The tandem PSC geometry dramatically impacts the pool of materials available for the realization of effi cient hole and , and a fi ll factor of 0.62 ± 0.01, resulting in a power conversion effi ciency of 6.5% ± 0.1% under simulated AM 1.5G, 100 mW cm −2 illumination.