Harmonic distortion is one of the dominant factors limiting the overall signal-to-noise and distortion ratio of seismic-grade sigma-delta MEMS accelerometers. This study investigates harmonic distortion based on the multiple degree-of-freedom model (MDM) established in our previous study. The main advantage of using an MDM is that the effect of finger flexibility on harmonic distortion is considered. Initially, the nonlinear relationship between the input acceleration and output signal is derived using the MDM. Then, harmonic distortion is simulated and described in terms of the nonlinear input–output relationship. It is found that finger flexibility and parasitic capacitance mismatch both decrease harmonic distortion. Finally, the experimental testing of harmonic distortion is implemented. By reducing the finger length to realize a higher stiffness and compensating for the parasitic capacitance mismatch, the total harmonic distortion decreases from −66.8 dB to −86.9 dB.