In recent decades, moisture evaluation of transformer oil-immersed cellulose insulation has been widely studied by using the frequency domain spectroscopy (FDS) technique. However, due to the difficulties in sample preparation, most of the existing evaluation methods are based on a small number of samples, which greatly limits the evaluation accuracy of these methods. To accurately evaluate moisture inside transformer oil-immersed cellulose insulation, a novel method combining the FDS technique and the exponential decay model is proposed. In current work, the exponential decay model is introduced to analyze the FDS data, which can be used to assess the quantitative relationship between moisture and extracted parameters. Then, the FDS curves with different moisture can be predicted by using these parameters to form a curve database. Findings reveal the relative error of evaluation results in lab condition is less than 10.57% when using the proposed curve database. In that respect, the feasibility of the proposed database is proved for moisture evaluation of transformer oil-immersed cellulose insulation.