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Cross-flow hollow fiber membranes are commonly applied in humidification/dehumidification. Hollow fiber membranes vibrate and deform under the impinging force of incoming air and the gravity of liquid in the inner tube. In this study, fiber deformation was caused by the pulsating flow of air. With varied pulsating amplitudes and frequencies, single-fiber deformation was investigated numerically using the fluid–structure interaction technique and verified with experimental data testing with a laser vibrometer. Then, the effect of pulsating amplitude and frequency on heat and mass transfer performance of the hollow fiber membrane was analyzed. The maximum fiber deformation along the airflow direction was far larger than that perpendicular to the flow direction. Compared with the case where the fiber did not vibrate, increasing the pulsation amplitude could strengthen <i>Nu</i> by 14–87%. Flow-induced fiber vibration could raise the heat transfer enhancement index from 13.8% to 80%. The pulsating frequency could also enhance the heat transfer of hollow fiber membranes due to the continuously weakened thermal boundary layer. With the increase in pulsating amplitude or frequency, the <i>Sh</i> number or <i>E</i>_m under vibrating conditions can reach about twice its value under non-vibrating conditions.