Lead halide perovskites are promising candidates for optoelectronic applications, as they combine a high absorption coefficient, a steep absorption onset, and a certain tolerance against defects with low-cost favorable manufacturing perspectives. [1][2][3][4] In particular, the rapid rise in perovskite solar cell efficiency from below 10% to over 25% in less than 10 years attracted international attention. [5,6] Currently, high-efficiency perovskite solar cells (PSCs) are typically prepared by solution-based processes, although evaporation techniques, which are widely used in the semiconductor industry, offer unique advantages. [7,8] In particular, vacuum processes enable the deposition of very smooth films and provide excellent control over film thickness and composition. [9] In addition, up-scaling to larger areas is feasible once the process control is realized. To monitor the evaporation process, quartz crystal microbalances (QCM) are commonly used. [7,10] Although the co-evaporation process for perovskites was already successfully demonstrated in 2013 [11] and recently enabled solar cell efficiencies of over 20%, [12][13][14] the implementation of this technology is constrained by its low reproducibility. [15] Especially the complex evaporation behavior of methylammonium iodide (MAI), which includes extreme pressure rise, low rate stability, and poor adhesion to the QCM, was repeatedly reported as a challenge in several publications over the past decade. [13,[16][17][18][19][20][21][22][23] Despite these challenges, MAI is an essential precursor material for the vapor-deposition of highly efficient PSCs, as the literature overview presented in Table S1, Supporting Information illustrates.The evaporation of MAI differs from a conventional directional evaporation process being more vapor-based was already demonstrated by Ono et al. in 2014. [16] To determine the composition of this nondirectional evaporating MAI vapor, which is also referred to as MAI gas, [24] mass spectrometry (MS) studies were carried out. [22,25] Analyzing MAI by thermogravimetry coupled with MS, Juarez-Perez identified iodomethane (CH 3 I) and ammonia (NH 3 ) as gaseous decomposition products. [25] In contrast, the most recent study by Baekbo et al. concludes that the main decomposition products of MAI are methylamine (CH 3 NH 2 ) and hydrogen iodide (HI). [22] Furthermore, it is suggested that for the conversion of the lead halide both compounds (HI and CH 3 NH 2 ) need to be present and a high chamber pressure is beneficial for a successful co-evaporation. [22] In accordance with these findings, high deposition pressures of 10 À4 -10 À3 mbar,