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Associations between frailty and physical-functional fitness (PFF) indicators in frail women over 65 years of age remain largely unexplored. This study analyzed the relationship between frailty syndrome (FS) and PFF indicators and assessed how the latter might predict the former. Participants were 119 elderly women (81.96 ± 7.89 years) recruited from four social and healthcare centers. PFF was assessed through muscle strength tests of upper and lower limbs, endurance, agility-dynamic balance, flexibility, and body composition. The following FS indicators were assessed: weight loss, exhaustion, weakness, slowness, and low physical activity level. Significant correlations were found between FS and endurance, agility-dynamic balance, upper and lower limbs muscle strength tests. Comparitive analyses also revealed that, among FS groups, the frail subgroup performed significantly poorer on all PFF measures except body composition. Additionally, a receiving operating characteristics curve analysis revealed good diagnostic accuracy for predicting FS using the agility-dynamic balance test (Area Under Curve [AUC] = .82, 95% CI [0.74, 0.90]; sensitivity and specificity were 70.4% and 84.8% for the cutoff = 16.22 seconds). Accurately, the risk of frail condition (not pre-frail) increases about 2.12% per second spent in this test. Thus, the agility-dynamic balance test is a promising tool for screening institutionalized older people for risk of FS.