Soil and water samples in and around the Long Valley geothermal area, Mono County, California, were collected and analyzed for helium by means of a modified mass spectrometer leak detector to see what relationship helium concentrations might have to geothermal features of the area, and to previously studied mercury anomalies in the area. Anomalously high concentrations of helium occurred over part of a major Sierra Nevada frontal fault and over other faults outside of the caldera. Anomalously low concentrations of helium occurred in several areas of high mercury concentrations, which were also areas of hydrothermal alteration. Quantities of helium exsolved from water samples did not fit any pattern.