Background: An increasing body of evidence indicates that the phase angle (PhA) can be applied as a marker of nutritional status, disease prognosis, and mortality probability. Still, it is not known whether PhA can be used as an indicator of muscular quantity and strength and maximal aerobic capacity in overweight/obese former highly active individuals, an understudied population. This study aimed to analyze the association between PhA with skeletal muscle mass, maximal isometric strength, and maximal aerobic capacity through VO2max, in overweight/obese and inactive former athletes. Methods: Cross-sectional information of 94 (62 males) former adult athletes (age: 43.1 ± 9.4 years old; body mass index: 31.4 ± 4.8 kg/m2) taking part in a weight-loss clinical trial was analyzed. Total fat and fat-free mass were determined by dual-energy X-ray absorptiometry, while skeletal muscle mass was predicted from appendicular lean soft tissue. Values for upper- and lower-body maximal isometric strength were assessed by handgrip and leg press dynamometry. VO2max was determined by indirect calorimetry through a graded exercise test performed on a treadmill. Results: PhA was associated with skeletal muscle mass (r = 0.564, p < 0.001), upper-body strength (r = 0.556, p < 0.001), lower-body strength (r = 0.422, p < 0.001), and VO2max (r = 0.328, p = 0.013). These relationships remained significant for skeletal muscle mass (β = 2.158, p = 0.001), maximal isometric strength (upper-body: β = 2.846, p = 0.012; low-er-body: β = 24.209, p = 0.041) after adjusting for age, sex, and fat mass but not for VO2max (β = −0.163, p = 0.098). Conclusion: Our findings indicated that former athletes with higher values of PhA exhibited greater muscle mass and strength, despite sex, age, and body composition, which suggests that this simple raw BI parameter can be utilized as an indicator of muscle quantity and functionality in overweight/obese former athletes.