both the top and bottom electrodes. These semitransparent PSCs (ST-PSCs) could be used as power generating windows and aesthetic architectural glasses, which are considered as the most appealing photovoltaic product for building integrated photovoltaic applications. [12][13][14][15][16][17][18] However, unlike opaque PSCs, the overall performance of ST-PSCs depends not only on the PCE but also the average visible transmittance (AVT) and color rendering properties. [19] Therefore, the great challenge for ST-PSCs is to achieve high PCE yet with good AVT and color rendering properties.Optimization of both the PCE and AVT in ST-PSCs is inherently challenging as these two performance parameters are difficult to optimize at the same time. The ideal optical condition for ST-PSC can be reached when the light passes through the device is only absorbed by the active layer but not the other layers such as the transparent electrodes and the interlayers, which allows the maximal amount of light transmitted through the devices. The ideal electronic condition for ST-PSC fulfilled if all the photons absorbed by the light harvesting layer can be dissociated and collected to generate photocurrent with internal quantum efficiency equal to 100%. [20] However, in real cases, the optical and electronic properties of the ST-PSCs are strongly affected by the choice of interlayers and transparent electrodes. For example, the interlayer not only can act as a charge selective layer to improve charge extraction in PSCs but also can act as an optical spacer that alters the optical field distribution within the device. [21] Depending on the choice of the transparent conductive material used for constructing the transparent electrode, it can be categorized as nonreflective or semireflective one. The latter case, which can be fabricated using ultrathin metal films (UTMFs) with the reflectance and transmittance depending on the thickness of the metal films, is of particular interest as it provides better flexibility in tuning the optical property of ST-PSCs. [22,23] However, the deposition of high quality and smooth UTMF, which is a prerequisite for achieving high transparency and conductivity, as top transparent conducting electrode for ST-PSCs is not straight forward and the film quality is strongly depending of the choice of underneath charge transport layer and deposition conditions. [24][25][26] In previous reports, tailored charge transport layers, such as a C 60 surfactant as electron transport layer (ETL) and MoS 2 as hole transport layer, had been In this study the thickness of the PTB7-Th:PC 71 BM bulk heterojunction (BHJ) film and the PF3N-2TNDI electron transport layer (ETL) is systematically tuned to achieve polymer solar cells (PSCs) with optimized power conversion efficiency (PCE) of over 9% when an ultrathin BHJ of 50 nm is used. Optical modeling suggests that the high PCE is attributed to the optical spacer effect from the ETL, which not only maximizes the optical field within the BHJ film but also facilitates the formation of a...