Plasma treatment was conducted to modify the outer-and inner-layer surfaces of bamboo in a multi-factor experiment, where the surface contact angles and surface energy were measured, followed by investigation on the surface microstructure and functional groups using a scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS), respectively. The result showed that when the power of the gliding arc plasma treatment was 1000 W while the bamboo surface was 3 cm away from the nozzle of the plasma thrower in the plasma flame, the contact angles of the outer-and inner-layer surfaces decreased, whereas the surface energy increased as a function of the treatment time. The 40 s treatment on the outer-layer surface caused the contact angle to reach 40 • , and the surface energy accomplished a value of 45 J. Likewise, when the inner-layer surface was exposed for 30 s treatment, its contact angle attained a value of 15 • , while the surface energy elevated to 60 J. Surface assessment with scanning electron microscopy (SEM) demonstrated etched microstructures of outer-and inner-layer surfaces of the bamboo culm after the treatment with gliding arc plasma. Moreover, the soaking test performed on the surfaces signified that 2D resin could have adhered more easily to outer-and inner-layer surfaces, which was considered a result of the greater uniformity and smoothness acquired after the treatment. X-ray photoelectron spectroscopic (XPS) analysis revealed that hydrophilic groups (O-CO-N, -NO 2− ,-NO 3− , C-O-C, C-O-H and O-CO-OH, C-O-C = O) emerged on outer-and inner-layer surfaces of bamboo culms after being treated by gliding arc plasma, which enhanced the interaction of bamboo culms with applied protective coating resins.