In January 2014, approximately 37 800 L of crude 4-methylcyclohexanemethanol (crude MCHM) spilled into the Elk River, West Virginia. To understand the long-term fate of 4-MCHM, we conducted experiments under environmentally relevant conditions to assess the potential for the 2 primary compounds in crude MCHM (1) to undergo biodegradation and (2) for sediments to serve as a long-term source of 4-MCHM. We developed a solid phase microextraction (SPME) method to quantify the cis- and trans-isomers of 4-MCHM. Autoclaved Elk River sediment slurries sorbed 17.5% of cis-4-MCHM and 31% of trans-4-MCHM from water during the 2-week experiment. Sterilized, impacted, spill-site sediment released minor amounts of cis- and up to 35 μg/L of trans-4-MCHM into water, indicating 4-MCHM was present in sediment collected 10 months post spill. In anoxic microcosms, 300 μg/L cis- and 150 μg/L trans-4-MCHM degraded to nondetectable levels in 8–13 days in both impacted and background sediments. Under aerobic conditions, 4-MCHM isomers degraded to nondetectable levels within 4 days. Microbial communities at impacted sites differed in composition compared to background samples, but communities from both sites shifted in response to crude MCHM amendments. Our results indicate that 4-MCHM is readily biodegradable under environmentally relevant conditions.