Burnishing experiments with different burnishing parameters were performed on a computer numerical control milling machine to characterize the surface roughness of an aluminum alloy during burnishing. The chaos theory was employed to investigate the nonlinear features of the burnishing system. The experimental results show that the power spectrum is broadband and continuous, and the Lyapunov exponent λ is positive, proving that burnishing has chaotic characteristics. The chaotic characteristic parameter, the correlation dimension D, is sensitive to the time behavior of the system and is used to establish the corresponding relationship with the surface roughness. The correlation dimension was the largest, when the surface roughness was the smallest. Furthermore, when the correlation dimension curve decreases, the roughness curve increases. The correlation dimension and surface roughness exhibit opposite variation trends. The higher the correlation dimension, the lower the surface roughness. The surface roughness of the aluminum alloy can be characterized online by calculating the correlation dimension during burnishing.