wide dissemination, and high technological throughput. [8] As a unique event in the landscape of solar energy harvesting, perovskite solar cells have experienced an increment of their power conversion efficiency by ≈8% (from 13.4% to 23.7%) in the last 5 years. [9,10] This technology is expected to successfully contribute to the enormous challenge of future power supply from sustainable energy sources. However, the well-known structural instability of hybrid perovskites under working conditions limits a real market uptake of all the related technologies. Solutions to guarantee the durability of products are mandatory and can be numerous, if the problem is addressed from different perspectives.Within the possible approaches to stabilize the perovskite lattice and its behavior under illumination, recent efforts have focused on introducing various treatments, [11,12] molecules, or additives, [13][14][15][16][17][18][19] through different procedures. Nitrogen has been also exploited as inert species [20][21][22][23][24] but its role is still unfocused. The existing (direct or indirect) findings in the literature stimulate the idea of beneficially using N 2 molecules in technological solutions, if their role is persuasively afforded. [25] N 2 molecules are small, safe, and easy to apply.Related to the material stability, we emphasize that the plethora of perovskites produced in different laboratories, with preparation procedures changing from lab to lab and from time to time, ask for treatments that take care and, in a certain extent, reset the starting conditions in a convenient and reproducible manner. This is particularly needed for small grained perovskite layers, on one hand used to implement pinhole-free coverages, but, on the other hand, offering extended lattice discontinuities due to the high surface to volume ratio. In addition to morphology and environment, temperature-related effects are unavoidable during device operation. [24,26] A rationalization of the phenomena needs to embody heating and thermal cycles to preserve the material integrity and/or the structural reversibility versus temperature.In this framework, we argue that nitrogen species have an active role in the stabilization of all the exposed methylammonium lead iodide (MAPbI 3 ) surfaces via their action at grain shells. This conclusion is independent of the particular On the basis of experiment and theory, a general paradigm is drawn that reconsiders N 2 not simply being an inert species but rather an effective healing gas molecule if entering a methylammonium lead iodide (MAPbI 3 ) layer. Nitrogen is soaked into polycrystalline MAPbI 3 via a postdeposition mild thermal treatment under slightly overpressure conditions to promote its diffusion across the whole layer. A significant reduction of radiative recombination and a concurrent increase of light absorption, with a maximum benefit at 80 °C, are observed. Concomitantly, the current of holes drawn from the surfaces with nanometer resolution through a biased tip is raised by a factor of 3 un...