Background: Current assessment standards in chronic limb-threatening ischemia (CLTI) focus on macrovascular function while neglecting the microcirculation. Multispectral near-infrared spectroscopy (NIRS) provides hemodynamic characteristics of the microcirculation (i.e., capillaries) and may be a powerful tool for monitoring CLTI and preventing extremity loss. The aims of this study were to (1) investigate the effects of lower limb revascularization on the microcirculation and (2) determine if macrovascular and microvascular assessments correlate. Methods: An observational, retrospective cohort study of 38 endovascular interventions in 30 CLTI subjects was analyzed pre- and post-intervention for arterial Doppler acceleration times (AcT; macrovascular) and NIRS metrics (microvascular). Pre-intervention ankle-brachial index (ABI) was also analyzed. Results: AcT significantly decreased (p = 0.009) while oxyhemoglobin (HbO) significantly increased (p < 0.04) after endovascular intervention, indicating treatment efficacy. However, macrovascular measurements (ABI, AcT) and NIRS metrics of oxygenation and perfusion did not correlate (p > 0.06, r2 < 0.15, n = 23) indicating that macro- and microvascular assessment are not congruent. Conclusion: These findings suggest that macrovascular and microvascular assessments can determine interventional efficacy in their corresponding vasculature. Their lack of correlation, however, suggests the need for simultaneous assessment as independent use may cause diagnostic information to be missed.