Recently released data by the National Oceanic and Atmospheric Administration show that year-on-year growth in global atmospheric methane concentrations is now the largest since intensive measurements began in 1983. Methane has been rising rapidly in the atmosphere since 2007. The acceleration over the last decade, including the observed surge in 2020, is not well understood. Understanding the rapid increases in atmospheric methane remains a “Grand Challenge” in climate science. In this publication commissioned by the American Geophysical Union, we document some of the major gaps in our understanding of methane science. We illustrate research priorities in the field over the next decade with the goal to finally tackle a puzzle that has been eluding scientists for more than a decade. This animation illustrates the complex sources and sinks that drive methane concentrations in the atmosphere and explains why unraveling methane emissions from human and natural systems is a complex research topic.