The National Fire Protection Association (NFPA) 1851 document provides guidelines for firefighters on the care and maintenance of their PPE, including decontamination practices. Firefighters are exposed to various toxic chemicals during fire suppression activities, making effective decontamination crucial for their safety. This study evaluated the efficacy of different washing parameters, including temperature, time, and surfactants, on cleaning outer-shell material contaminated with nine targeted compounds from three different functional groups: phenols, polycyclic aromatic hydrocarbons (PAHs), and phthalates. The study was conducted on both bench-scale and full-scale levels, with contaminated swatches washed in a water shaker bath in the bench-scale evaluation and full-sized washer extractors used in the full-scale evaluation. The results showed that bench-scale washing demonstrated similar trends in contaminant removal to full-scale washing. Importantly, the study highlighted the complexity of removing fireground contaminants from the personal protective ensemble (PPE). The findings of this study have practical implications for the firefighting industry as they provide insight into the effectiveness of different washing parameters for PPE decontamination. Future studies could explore the impact of repeated washing on PPE and investigate the potential for developing more efficient decontamination strategies. Ultimately, the study underscores the importance of ongoing efforts to ensure the safety of firefighters, who face significant occupational hazards.