well-established state-of-the-art devices such as silicon heterojunction solar cells and inorganic and organic light-emitting diodes (LEDs) to perovskite solar cells (PSCs), and organic solar cells. [5][6][7][8] There are also many examples of TCOs in new approaches that simultaneously require semitransparency and flexibility, such as semitransparent conductors, field-effect transistors, thermal shields, photo-detectors, and vertical transistors. [9][10][11][12][13][14] PSCs have attracted much interest since their onset in 2009 due to rapidly-increasing power conversion efficiencies (currently above 25% for small area cells). The perovskite layer and any adjacent charge transport layers can be fabricated in many ways using either solution-based processes or vacuum-assisted deposition. Vacuum-based deposition has the advantage of better control over the film thickness and is an additive method, moreover, it is a widely employed method of production of the before mentioned opto-electronic devices. [15,16] Despite the benefits and promising perspectives of using TCOs in optoelectronics, the development of organic/TCO (TCO on top of organic) bi-layer structures is still a non-trivial challenge because of the generally harsh processing conditions involved in the deposition of the TCO layers. [17] For both lab-and industrial-scale deposition of TCO, magnetron sputtering is the most widespread technique. It is a vacuumbased process that employs direct current or radio frequency to excite a carrier gas (most commonly Ar) into a high kinetic energy plasma which bombards a target material, resulting in the transfer of fragments from the target to substrates positioned above it. However, the accelerated particles, together with side phenomena such as plasma luminescence and processing-induced heat, can easily damage soft organic semiconductor layers, leading to increased leakage current, as well as reduced efficiency and a lower lifetime of the optoelectronic device. [18,19] To overcome this limitation, a protective buffer layer is deposited prior to the TCO deposition. [17] Also, many efforts were proposed to minimize damages of sputtering deposition on buffer-layer-free stacks by lowering the power density threshold by changes in power, target to substrate distance, sputtering gas, and process pressure, [20][21][22][23][24] but at the expense of longer processing times. [22,[25][26][27][28][29] Among these reports, the most efficient buffer-layer-free PSC using TCO top-electrode was achieved by Ramos et al. employing a post-annealed ITO sputtered directly onto a thick (290 nm) spiro-OMeTAD hole The deposition of transparent conductive oxides (TCO) usually employs harsh conditions that are frequently harmful to soft/organic underlayers. Herein, successful use of an industrial pulsed laser deposition (PLD) tool to directly deposit indium tin oxide (ITO) films on semitransparent vacuum-deposited perovskite solar cells without damage to the device stack is demonstrated. The morphological, electronic, and optical properties o...