Coronary heart disease (CHD) remains a significant global health concern, with exercise therapy playing a crucial role in rehabilitation. Optimizing exercise intensity is essential, as both insufficient and excessive exercise may lead to suboptimal or adverse outcomes. In response to this challenge, we developed Adaptive Posture-Balance Cardiac Rehabilitation Exercise (APBCRE), which integrates postural balance training with aerobic exercise. To evaluate its therapeutic efficacy, we designed a novel fluorescent biosensor targeting soluble vascular cell adhesion molecule-1 (sVCAM-1), a key biomarker of endothelial inflammation. The biosensor utilizes pyrene-functionalized metal–organic framework (PCA-UiO-66), synthesized via a one-pot approach. Within the MOF, pyrenecarboxylic acid (PCA) exists primarily in the excimer state, exhibiting stable fluorescence emission, a narrow spectral peak, and a wide Stokes shift. For the purpose of identify sVCAM-1, the sVCAM-1-specific aptamer was functionalized to PCA-UiO-66. When sVCAM-1 is present, the aptamer is competitively stripped from the MOF surface by the target. This process induces π–π stacking interactions between the aptamer's phosphate backbone and PCA molecules, facilitating PCA release and transition from the excimer to the monomer state. By quantifying the fluorescence value of monomer state PCA, the fluorescence response allowed precise quantification of sVCAM-1, with a detection limit of 0.69 ng/mL and a range of 2 ng/mL to 50 μg/mL. We analyzed cardiopulmonary performance and serum sVCAM-1 levels in 20 CHD patients who underwent APBCRE. These findings establish APBCRE as an effective rehabilitation strategy that provides both physiological and molecular benefits while also confirming Apt@PCA-UiO-66 as a robust biosensing tool for monitoring therapeutic efficacy and elucidating CHD pathophysiology.