In this study, the external load resistance of a magnetically coupled two-degree-of-freedom bistable energy harvester (2-DOF MCBEH) was optimized to maximize the harvested power output, considering the third-harmonic distortion in forced response. First, the nonlinear dynamic analysis was performed to investigate the characteristics of the large-amplitude interwell motions of the 2-DOF MCBEH. From the analysis results, it was found that the third-harmonic distortion occurs in the interwell motion of the 2-DOF MCBEH system due to the nonlinear magnetic coupling between the beams. Thus, in this study, the third-harmonic distortion was considered in the optimization process of the external load resistance of the 2-DOF MCBEH, which is different from the process of conventional impedance matching techniques suitable for linear systems. The optimal load resistances were estimated for harmonic and swept-sine excitations by using the proposed method, and all the results of the power outputs were in excellent agreements with the numerically optimized results. Furthermore, the associated power outputs were compared with the power outputs obtained by using the conventional impedance matching technique. The results of the power outputs are discussed in terms of the improvement in energy harvesting performance.