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(1) Background: AliveCor KardiaMobile (KM) is a portable electrocardiography recorder for detection of atrial fibrillation (AF). The aim of the study was to define the group of acute ischemic stroke (AIS) patients who can use the KM device and assess the diagnostic test accuracy. (2) Methods: the AIS patients were recruited to the study. Thirty-second single-lead electrocardiogram (ECG) usages were recorded on demand for three days using KM portable device. Each KM ECG record was verified by a cardiologist. The feasibility was evaluated using operationalization criteria. (3) Results: the recruitment rate among AIS patients was 26.3%. The withdrawal rate before the start of the intervention was 26%. The withdrawal rate after the start of the intervention was 6%. KM device detected AF in 2.8% of AIS patients and in 2.2% of ECG records. Cardiologist confirmed the AF in 0.3% AIS patients. Sensitivity and specificity of KM for AF was 100% and 98.3%, respectively. (4) Conclusions: the results of this study suggest that it is feasible to use KM device to detect AF in the selected AIS patients (younger and in better neurological condition). KM detected AF in the selected AIS patients with high specificity and sensitivity.