single solution, which is deposited onto the substrate, following by a thermal annealing step. [6,7] While this approach is very simple and is still relatively common for certain perovskite compositions, [8,9] the perovskite precursors maybe undergo various chemical reactions in solution, which will influence both the resulting film and the performance of photovoltaic devices. [10] An alternative approach, especially popular in the early days of perovskite research, is the two-step approach, in which one of the precursors is deposited first, followed by the deposition of a second precursor and thermal annealing. [11] Most commonly, the first precursor (e.g., lead iodide, PbI 2) is deposited by spin-coating, while the second one (e.g., methylammonium iodide, MAI) can be deposited by dipping the sample into a solution, [12] or by spin-coating on top of the first layer. [13] For a time, devices fabricated using the two-step method showed higher performance than those made using the one-step, [14] but the situation drastically changed upon the introduction of the solvent engineering approach, [15] which remains the most commonly used to date. This method is a modification of the one-step approach, with all perovskite precursors deposited in a single step, during which an antisolvent is applied triggering the crystallization of the perovskite film. [16] Similarly, several variations of deposition of perovskite layers by thermal evaporation have also been demonstrated. These include the single-source evaporation, sequential evaporation and multiple source coevaporation (Figure 1). Single-source evaporation is possible either via combining the perovskite precursors into a single crucible [17] or by first preparing (e.g., via solution-processing) perovskite crystals that are ground into a powder for evaporation. [18] Sequential evaporation follows a similar approach to that of the two-step solution-processed deposition, with each precursor evaporated separately, following by a thermal or vapor annealing. [19] The most common approach, however, is based on the multisource evaporation, in which each precursor is loaded into a separate crucible and is coevaporated along with all other precursors to form the perovskite layer. Importantly, unlike solution-processed perovskite films, it is possible to form crystalline perovskite layers by thermal evaporation without annealing; [20] however, many studies still rely on annealing for improving the evaporated films' properties. [21,22] It is noteworthy that many additional methods for the deposition of perovskite films exist such as inkjet printing, [23] spray coating, [24] chemical vapor deposition, [25] flash evaporation, [26] and many others; [27] however, these methods are less common in literature and generally show lower performance than those fabricated by the methods outlined above. The last decade has seen remarkable advancements in the field of perovskite materials and photovoltaic technologies. One of their most extraordinary characteristics is the high quality of layer...