This study provides a novel method for improving the anaerobic digestion (AD) of Holstein dairy manure (HDM) by the direct addition of Mineraso (MnS), a natural soil-derived supplement, to the feed of Holstein dairy cattle (HDC). MnS is chiefly composed of approximately 69.08% Fe3O4 and was supplemented at rates of 0 (F1), 25 (F2), and 50 (F3) g/head of HDC/d for two months. The HDM was then examined for non-absorbed iron prior to the batch and semi-continuous bench AD experiments. The results revealed that MnS enhanced CH4 generation in F2 and F3 by 25% and 42%, respectively, in the batch experiments compared to that of F1. Additionally, the gas yield improved in F2 and F3 by 45% and 66%, respectively, over the control after 7 d in the bench experiments. Therefore, supplementing animals with MnS represents a sustainable and economic approach to enhancing CH4 yields.