Commercially available Jeffamines (polyetheramine) with average molecular weights of 2000 and 3000 g mol-1; one (M2005), two (D2000), and three (T3000) primary amino groups end-capping on the polyether backbone; and propylene oxide (PO) and ethylene oxide (EO) functionality were explored as additives for application in MAPbI3 perovskite solar cells (PSCs). The results indicated that the embedding of Jeffamine additives effectively passivates the defects in the grain boundaries of perovskite through the coordination bonding between the nitrogen atom and the uncoordinated lead ion of perovskite. We fabricated p-i-n PSC devices with the structure of glass/indium tin oxide (ITO)/NiOx/CH3NH3PbI3 (with and without Jeffamine)/PC61BM/BCP/Ag. We observed the interaction between the Jeffamine and perovskites. This interaction led to increased lifetimes of the carriers of perovskite, which enabled the construction of high-performance p-i-n PSCs. For the Jeffamine-D2000-derived device, we observed an increase in the power conversion efficiency from 14.5% to 16.8% relative to the control device. Furthermore, the mechanical properties of the perovskite films were studied. The interaction between the additive and perovskite reinforced the flexibility of the thin film, which may pave the way for stretchable optoelectronics.