As a fast and non-destructive spectroscopic analysis technique, Raman spectroscopy has been widely applied in chemistry. However, noise is usually unavoidable in Raman spectra. Hence, denoising is an important step before Raman spectral analysis. A novel spectral denoising method based on variational mode decomposition (VMD) was introduced to solve the above problem. The spectrum is decomposed into a series of modes (uk) by VMD. Then, the high-frequency noise modes are removed and the remaining modes are reconstructed to obtain the denoised spectrum. The proposed method was verified by two artificial noised signals and two Raman spectra of in-organic materials, i.e., MnCo ISAs/CN and Fe-NCNT. For comparison, empirical mode decomposition (EMD), Savitzky–Golay (SG) smoothing, and discrete wavelet transformation (DWT) are also investigated. At the same time, signal-to-noise ratio (SNR) was introduced as evaluation indicators to verify the performance of the proposed method. The results show that compared with EMD, VMD can significantly improve mode mixing and the endpoint effect. Moreover, the Raman spectrum by VMD denoising is more excellent than that of EMD, SG smoothing and DWT in terms of visualization and SNR. For the small sharp peaks, some information areis lost after denoising by EMD, SG smoothing, DWT and VMD while VMD losest fewest information. Therefore, VMD may be an alternative method for Raman spectral denoising.