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In the present study, the influence of friction stir processing (FSP) tool rotational speed and tool travel speed on achieving higher hardness in ZE41 Mg alloy was investigated by adopting a Taguchi design model using orthogonal array. The extent of grain refinement, hardness enhancement, and achieving defect-free stir zones in FSP completely depend on process parameters. In the present work, FSP parameters such as tool rotation speed and tool traverse speed were varied. The microscopic and macroscopic observations revealed that tool speeds of 1,400 rpm with 25 and 50 mm/min feeds were found to be optimal to develop fine grain size and wide stir zone, respectively, without defect. These results are in good agreement with the design model and help with choosing optimized parameters with a minimum number of experiments in developing grain-refined ZE41 Mg alloy for emerging lightweight technological applications.