We examined the association of cardiorespiratory fitness with metabolic syndrome in overweight/obese postmenopausal African-American women. Pooled baseline data on 170 African- American women from two exercise trials were examined. Metabolic syndrome was defined as at least three of the following: abdominal obesity, glucose intolerance, hypertension, low high-density lipoprotein cholesterol (HDL-C), and high triglycerides. Cardiorespiratory fitness (VO2peak) was determined using the Bruce treadmill protocol and categorized as: Very Low (VLCRF < 18 mL·kg−1 ·min−1), Low (LCRF = 18.0 – 22.0 mL·kg−1 ·min−1), and Moderate (MCRF > 22.0 mL·kg−1 ·min−1). Associations of metabolic syndrome with cardiorespiratory fitness were analyzed using one-way ANOVA and linear regression. VO2peak was significantly lower in the VLCRF compared to the MCRF group. Lower cardiorespiratory fitness was associated with higher prevalence of metabolic syndrome, abdominal obesity, hypertriglyceridemia, and low HDL among overweight/obese postmenopausal African-American women. In fully adjusted models, higher waist circumference and triglycerides were associated with lower VO2peak levels (P < 0.01) and higher HDL-C was associated with higher VO2peak levels (P = 0.03). Overweight/obese postmenopausal African-American women with very low cardiorespiratory fitness are more likely to have metabolic syndrome, higher body mass index, and unhealthier levels of certain metabolic syndrome components than women with moderate cardiorespiratory fitness.