A new vector matching balance method (VMBM) based on the identification of energy transfer coefficient of spindle rotor system (ETCSRS) is proposed in this paper. This method only needs to extract the original vibration signal of the spindle to compute the spindle rotor system unbalanced vector, and the calculation accuracy depends on the identification precision of ETCSRS. The initial parameters of bearings were calculated by applying Newton-Raphson algorithm based on the quasi-static mechanics analysis of rolling bearings. Through establishing the FEA model of spindle, the structural parameters of the rotor shaft system are obtained and modified by modal correction method. First, the principle of VMBM is verified on a Bentley rotor test bench at different rotating speeds. Second, the verification experiment of VMBM on a high-speed spindle is carried out. Furthermore, the VMBM has a better performance than the influence coefficient method (ICM). The method proposed in this paper is very suitable for on-line dynamic balancing, since it greatly improves the balance efficiency.