Seed-induced multistep and one-step hydrothermal methods have been successfully used by Lee et al. [ 31 ] and Wu et al. [ 15 ] to fabricate hyperbranched TiO 2 nanostructures with improved light harvesting in DSSCs owing to their larger surface area. However, these synthesis methods have resulted in a low density of nanofi bers, [ 15,31 ] and have suffered from slow carrier transport due to the presence of structural defects, including at grain boundaries between the nanofi ber trunks and nanorod branches of the hyperbranched ETM. Electrospinning of metal oxide nanofi bers has recently emerged as a potentially inexpensive, rapid, facile, and versatile route to growing 1D TiO 2 nanomaterials on a variety of substrates, [ 40,41 ] and has been investigated as a 1D material in the context of DSSCs. [42][43][44] However, the combination of electrospun TiO 2 fi bers with hydrothermally grown TiO 2 branches has not been investigated in the contexts of DSSCs or PSCs. [ 45 ] In this communication, we introduce a unique and scalable multistage electrospinning and hydrothermal route for the development of 3D hyperbranched anatase TiO 2 nanorodnanofi ber arrays as electron transporting materials. The hyperbranched ETM with optimal electron transport and carrier lifetime leads to highly effi cient mesostructured perovskite (CH 3 NH 3 PbI 3 ) solar cells with an average power conversion effi ciency (PCE avg ) of 15.03% and a maximum power conversion effi ciency (PCE max ) of 15.50%. Increasing the thickness of the hyperbranched ETM from 0.6 µm to ≈29 µm led to highly effi cient DSSCs as well, with PCE max = 11.22%. These remarkable performances were possible thanks to the development of 3D hyperbranched nanofi ber-nanorod arrays made of high quality anatase TiO 2 with few defects and capable of transporting electrons rapidly and over long distances, minimizing recombination losses. Light harvesting was also found to be signifi cantly enhanced due to light scattering effects of the hyperbranched architecture, leading to signifi cant performance boosts in DSSCs. This work demonstrates remarkable advantages in using hyperbranched ETMs for highly effi cient, largearea, and low-cost hybrid photovoltaics.In Figure 1 a, we show scanning electron micrographs (SEM) of nanofi bers obtained by electrospinning of a fi rst layer without subsequent hydrothermal synthesis of nanorod branches (E 1 H 0 ). We have carefully selected the electrospinning conditions, such as the applied voltage, the solution viscosity, and fl ow rate, in order to obtain nanofi bers assembled from small TiO 2 nanoparticles (40-50 nm diameter) and exhibiting significant internal porosity within the nanofi bers (see the Supporting Information). The formation of mesoporous nanofi bers is also an important requirement to obtaining hierarchically mesostructured nanofi ber-nanorod arrays during the subsequent Solution-processed hybrid thin fi lm photovoltaic technologies, such as perovskite solar cells (PSCs), dye sensitized solar cells (DSSCs), and colloidal quantum dot...