AbstractCardiovascular diseases are the leading cause of death globally; fortunately, 90% of cardiovascular diseases are preventable by long‐term monitoring of physiological signals. Stable, ultralow power consumption, and high‐sensitivity sensors are significant for miniaturized wearable physiological signal monitoring systems. Here, this study proposes a flexible self‐powered ultrasensitive pulse sensor (SUPS) based on triboelectric active sensor with excellent output performance (1.52 V), high peak signal‐noise ratio (45 dB), long‐term performance (107 cycles), and low cost price. Attributed to the crucial features of acquiring easy‐processed pulse waveform, which is consistent with second derivative of signal from conventional pulse sensor, SUPS can be integrated with a bluetooth chip to provide accurate, wireless, and real‐time monitoring of pulse signals of cardiovascular system on a smart phone/PC. Antidiastole of coronary heart disease, atrial septal defect, and atrial fibrillation are made, and the arrhythmia (atrial fibrillation) is indicative diagnosed from health, by characteristic exponent analysis of pulse signals accessed from volunteer patients. This SUPS is expected to be applied in self‐powered, wearable intelligent mobile diagnosis of cardiovascular disease in the future.