Passive microwave frequency (~300 MHz to 300 GHz) observations of the Moon have a long history and have been suggested as a plausible orbital instrument for the Moon and other bodies. However, global, orbital multifrequency measurements of lunar passive microwave emission have only recently been made by the Chinese Chang'E‐1 and ‐2 microwave radiometer (MRM) instruments. These missions carried nearly identical 4‐channel (3.0, 7.8, 19.35, and 37 GHz) instruments into lunar orbit in 2007–2009 and 2010–2011, respectively. Over the same time period, the ongoing Lunar Reconnaissance Orbiter (LRO) mission carried the Diviner Lunar Radiometer, which collected surface temperature measurements in the far infrared (~7.8–400 μm) from 2009 to present. By combining these data and associated thermal models, we provide new constraints on the relationship between physical temperature and microwave brightness temperature to reveal novel information about regolith thermal and dielectric properties which can reveal unique geologic information about the Moon. Here, we describe several first‐order global results to come from this combined data set, focusing primarily on the ability to detect, map, and quantify dielectric loss tangent variations of the Moon, including those from the presence of titanium‐bearing ilmenite. We update the loss tangent models for both highlands and mare and identify a clear frequency dependence that differs in sign between the two. We use the correlation with visible wavelength TiO2 mapping to provide a means to separate out the loss from rocks and from that of composition.