In this study, lab-scale, bench-scale, and pilot-scale experiments were carried out to optimize short-chain fatty acids production from primary sludge. Batch tests showed the requirement of short retention times and semi-continuous operation mode showed a plateau of maximum daily productivity at 36-hours hydraulic retention time with minimal methanation. Optimization from pH 5 to pH 10 at 36 h-hydraulic retention time under long-term semi-continuous operating mode revealed that production of short-chain fatty acids was pH dependent and highest yields could be achieved at pH 7 by establishing optimum redox conditions for fermentation. Pilot-scale experiments at 32 °C showed that daily productivity (3.1 g∙Lreactor-1∙dHRT-1) and yields (150 mg∙gVS-1; OLR = 21 gVS∙Lreactor-1∙dHRT-1; pH 7) of short-chain fatty acids could be significantly improved, specifically for acetic and propionic acids. From these results, a robust dark fermentation step for recovery of valuable products from the solids treatment step in a biorefinery can be achieved.