Pure sulfide CIGS solar cells are interesting candidates for standalone solar cells or top cells in a tandem configuration. To understand the limits and improve the power conversion efficiency of these devices, a comprehensive approach aimed at composition, interface, and process engineering should be employed. Here, the latter was explored. Using a two-step fabrication technique and one-variable-at-a-time methodology, we found the four processing factors affecting the absorber the most. While two were already backed by the previous literature, we found new and statistical evidence for two other important factors as well. The impact of alkali barrier diffusion was also established with statistical significance and under various processing conditions. Furthermore, the absorber roughness for samples without a barrier indicated a significant negative linear correlation with the devices’ efficiency. This contribution could aid engineers in more efficient process designs.