In this paper, we present measurements of He+ and He+2 ion‐induced sputtering of an anorthite‐like thin film at a fixed solar wind‐relevant impact energy of ~0.5 keV/amu using a quartz crystal microbalance approach (QCM) for determination of total absolute sputtering yields. He+2 ions are the most abundant multicharged ions in the solar wind, and increased sputtering by these ions in comparison to equivelocity He+ ions is expected to have the biggest effect on the overall sputtering efficiency of solar wind impact on the Moon. Our measurements indicate an almost 70% increase of the sputtering yield for doubly charged incident He ions compared to that for same velocity He+ impact (14.6 amu/ion for He+2 vs. 8.7 amu/ion for He+). Using a selective sputtering model, the new QCM results presented here, together with previously published results for Ar+q ions and SRIM results for the relevant kinetic‐sputtering yields, the effect due to multicharged‐solar‐wind‐ion impact on local near‐surface modification of lunar anorthite‐like soil is explored. It is shown that the multicharged‐solar‐wind component leads to a more pronounced and significant differentiation of depleted and enriched surface elements as well as a shortening of the timescale over which such surface‐compositional modifications might occur in astrophysical settings. In addition, to validate previous and future determinations of multicharged‐ion‐induced sputtering enhancement for those cases where the QCM approach cannot be used, relative quadrupole mass spectrometry (QMS)‐based measurements are presented for the same anorthite‐like thin film as were investigated by QCM, and their suitability and limitations for charge state‐enhanced yield measurements are discussed.