Halides play an important role in atmospheric chemistry, corrosion of steel, and also in controlling the abundance of O₃. Moreover high-precision vibrational energy spectra contain a large amount of quantum information of molecular system and are basic data for people to understand and manipulate molecules. At present, ab-initio methods have achieved many calculation results of the potential energy surfaces and corresponding vibrational energy of molecules, but they still face challenges in terms of accuracy and computational cost. Recently, data-driven machine learning methods have demonstrated very strong capability of extracting high-dimensional functional relationships from massive data and have been widely used in spectrum studies. ​Therefore, a theoretical approach to combining ab-initio method and machine learning algorithm is presented here to predict the vibrational energy of diatomic systems, which improves the accuracy and simultaneously reduces the computational cost. Firstly, the vibrational energy levels of 42 diatomic molecules are obtained by using different CCSD(T) methods to calculate the configurations from simple to complex and the corresponding experimental results are also collected. ​A machine learning algorithm is then used to learn the difference between the CCSD(T) method calculated vibrational results and the experimental vibrational results, and a high-dimensional error function is finally constructed to improve the original CCSD(T) computational accuracy. The results for HF, HBr, H³⁵Cl and Na³⁵Cl (they did not appear in the training set) and other halogen molecules show that compared with the CCSD(T)/cc-pV5Z calculation method alone, the present method reduces the prediction error by more than 50% and the computational cost by nearly one order of magnitude. It is worth noting that the method proposed in this paper is not only limited to the energy level prediction of diatomic systems, but also applicable in other fields where data can be obtained by ab initio methods and experimental methods simultaneously, such as the energy spectrum properties of macromolecular systems.