In this study, we demonstrated that the nonenzymatic glucose sensor based on the flexible carbon fiber bundle electrode with BDD nanocomposites (CF-BDD electrode). As a nano seeding method for the deposition of BDD on flexible carbon fiber, electrostatic self-assembly technique was employed. Surface morphology of BDD coated carbon fiber electrode was observed by scanning electron microscopy. And the electrochemical characteristics were investigated by cyclic voltammetry, electrochemical impedance spectroscopy and chronoamperometry. This CF-BDD electrode exhibited a large surface area, a direct electron transfer between the redox species and the electrode surface and a high catalytic activity, resulting in a wider linear range (3.75~50 mM), a faster response time (within 3 s) and a higher sensitivity (388.8 nA/mM) in comparison to a bare CF electrode. As a durable and flexible electrochemical sensing electrode, this brand new CF-BDD scheme has promising advantages on various electrochemical and wearable sensor applications.