Background: Metabolic syndrome (MetS) is a cluster of risk factors for cardiovascular disease, atherosclerosis and diabetes mellitus type 2 which may be reduced by practicing regular physical activity. Objective: To assess the leisure-time physical activity (LTPA) of older adults with MetS and without MetS. Methods: Cross-sectional study of older adults (55–80 years old) from Balearic Islands (Spain) with MetS (n = 333; 55% men) and without MetS (n = 144; 43.8% men). LTPA was assessed with the validated Spanish version of the Minnesota LTPA Questionnaire. Two criteria of physically active were used: >150 min/week of moderate physical activity or >75 min/week of vigorous physical activity or a combination of both, and total leisure-time energy expenditure of >300 MET·min/day. Sociodemographic and lifestyle characteristics, anthropometric variables, MetS components, and adherence to the Mediterranean diet (MD) were also measured. Results: MetS subjects showed lower energy expenditure in LTPA, lower adherence to the MD, higher obesity and waist circumference, and were less active than non-MetS peers. LTPA increased as participants got older and there was higher LTPA intensity as educational level increased. Adherence to MD was as high as LTPA was. Conclusions: MetS is associated with physical inactivity and unhealthy diet. To increase LTPA recommendations and raise awareness in the population about the health benefits of PA and high adherence to MD is highly recommended.