In recent years, flexible sensors based on laser-induced graphene (LIG) have played an important role in areas such as smart healthcare, smart skin, and wearable devices. This paper presents the fabrication of flexible sensors based on LIG technology and their applications in human–computer interaction (HCI) systems. Firstly, LIG with a sheet resistance as low as 4.5 Ω per square was generated through direct laser interaction with commercial polyimide (PI) film. The flexible sensors were then fabricated through a one-step method using the as-prepared LIG. The applications of the flexible sensors were demonstrated by an HCI system, which was fabricated through the integration of the flexible sensors and a flexible glove. The as-prepared HCI system could detect the bending motions of different fingers and translate them into the movements of the mouse on the computer screen. At the end of the paper, a demonstration of the HCI system is presented in which words were typed on a computer screen through the bending motion of the fingers. The newly designed LIG-based flexible HCI system can be used by persons with limited mobility to control a virtual keyboard or mouse pointer, thus enhancing their accessibility and independence in the digital realm.