Organo-lead halide perovskites have emerged as promising light harvesting materials for solar cells. The ability to prepare high quality films with a low concentration of defects is essential for obtaining high device performance. Here, we advance the procedure for the fabrication of efficient perovskite solar cells (PSCs) based on mechanochemically synthesized MAPbI3. The use of mechano-perovskite for the thin film formation provides a high degree of control of the stoichiometry and allows for the growth of relatively large crystalline grains. The best device achieved a maximum PCE of 17.5% from a current–voltage scan (J–V), which stabilized at 16.8% after 60 s of maximum power point tracking. Strikingly, PSCs based on MAPbI3 mechanoperovskite exhibit lower “hysteretic” behavior in comparison to that comprising MAPbI3 obtained from the conventional solvothermal reaction between PbI2 and MAI. To gain a better understanding of the difference in J–V hysteresis, we analyze the charge/ion accumulation mechanism and identify the defect energy distribution in the resulting MAPbI3 based devices. These results indicate that the use of mechanochemically synthesized perovskites provides a promising strategy for the formation of crystalline films demonstrating slow charge recombination and low trap density.