Objective. Epidemiologic studies suggest an inverse relationship between nonalcoholic fatty liver disease (NAFLD), visceral adipose tissue (VAT), and self-reported physical activity levels. However, subjective measurements can be inaccurate and prone to reporter bias. We investigated whether objectively quantified physical activity levels predicted liver fat and VAT in overweight/obese adults. Methods. Habitual physical activity was measured by triaxial accelerometry for four days (n = 82). Time spent in sedentary behavior (MET < 1.6) and light (MET 1.6 < 3), moderate (MET 3 < 6), and vigorous (MET 6 < 9) physical activity was quantified. Magnetic resonance imaging and spectroscopy were used to quantify visceral and liver fat. Bivariate correlations and hierarchical multiple regression analyses were performed. Results. There were no associations between physical activity or sedentary behavior and liver lipid. Sedentary behavior and moderate and vigorous physical activity accounted for just 3% of variance for VAT (p = 0.14) and 0.003% for liver fat (p = 0.96). Higher levels of VAT were associated with time spent in moderate activity (r = 0.294, p = 0.007), but there was no association with sedentary behavior. Known risk factors for obesity-related NAFLD accounted for 62% and 40% of variance in VAT and liver fat, respectively (p < 0.01). Conclusion. Objectively measured levels of habitual physical activity and sedentary behavior did not influence VAT or liver fat.