We demonstrate nontoxic, earth-abundant lightabsorbing SnS thin films fabricated by a low-cost, environmentally friendly nonvacuum process. SnS nanocrystals (NCs) are mechanochemically synthesized from elemental powders without the use of any other additives or solvents. To investigate the effect of the Sn-to-S stoichiometric ratio on the crystalline phase of the SnS NCs, the nonstoichiometry is systematically controlled from 0.95 (Sn 0.95 S) to 1.05 (Sn 1.05 S) by adjusting the mixing ratio of the Sn and S powders. The crystallographic evolution with the milling time signifies that the formation of the SnS phase follows a mechanochemically driven self-propagation reaction mechanism. The as-synthesized SnS NCs with a stoichiometric composition (i.e., Sn 1.00 S) are found to contain a Sn 2 S 3 impurity phase in a nonnegligible amount, which can be subsequently eliminated by a post heat treatment at 500 °C in a reducing atmosphere. Interestingly, however, the formation of Sn 2 S 3 during the mechanochemical synthesis process is greatly alleviated by introducing a Sn-excess composition (e.g., Sn 1.05 S). In addition, the solar cell with a Sn 1.05 S absorber exhibits a much higher efficiency as compared to the Sn 0.95 S-or Sn 1.00 S-based devices, which is likely attributed to the improved phase purity of Sn-excess SnS as well as to its better microstructure with higher crystallinity than the other compositions.