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In this paper, three new important aspects of rotary electromagnetic vibration energy harvesting technology (RE-VEH) are concerned and investigated: (i) vibro-electric coupling mechanism of the RE-VEH system is studied through theoretical modeling; (ii) quantitative analysis of system parameters based on numerical simulation method is carried out for the optimal design of RE-VEH; and (iii) dynamic power output performance of the RE-VEH system in free vibration is discussed. The parameter adjusting methods of the RE-VEH system in free vibration mode are obtained through theoretical analysis and numerical simulation. The experimental results show that the power output performance of RE-VEH in free vibration mode matches the numerical simulation results. The simulation and experimental results show that the maximum voltage output and power output of the RE-VEH with different structure parameters under free vibration can be up to the level of 100∼101 V/watt. The above results indicate that RE-VEH in a free vibration environment has significant energy output performance.