Ground-penetrating radar (GPR) is an effective tool for subsurface detection. Due to the influence of the environment and equipment, the echoes of GPR contain significant noise. In order to suppress noise for GPR data, a method based on singular value decomposition (SVD) of a window-length-optimized Hankel matrix is proposed in this paper. First, SVD is applied to decompose the Hankel matrix of the original data, and the fourth root of the fourth central moment of singular values is used to optimize the window length of the Hankel matrix. Then, the difference spectrum of singular values is used to construct a threshold, which is used to distinguish between components of effective signals and components of noise. Finally, the Hankel matrix is reconstructed with singular values corresponding to effective signals to suppress noise, and the denoised data are recovered from the reconstructed Hankel matrix. The effectiveness of the proposed method is verified with both synthetic and field measurements. The experimental results show that the proposed method can effectively improve noise removal performance under different detection scenarios.