A method, apparatus and system for controlling a smart device based on a headphone are disclosed. The method includes: collecting, by the headphone, head motion feature data of a human body if a trigger condition of a collection task is satisfied; judging, according to the collected data, whether a target motion feature satisfying a predetermined motion feature is present in head motion feature of the human body; and if the target motion feature is present, acquiring information of an application currently running on the smart device, and generating an operation control instruction corresponding to the target motion feature according to the information of the currently running application and sending the operation control instruction to the smart device. According to the present application, control function may be enhanced for the smart device and control accuracy may be improved.