In article number 1905892, Robert F. Klie and co‐workers show that alloy engineering can be used to control the thermal expansion (TEC) of 2D materials, including the transition metal dichalcogenide Mo1−xWxS2. Using a combination of atomic‐resolution scanning transmission electron microscopy imaging and electron spectroscopy at elevated temperature with first‐principles modeling, the dependence of the TEC on the chemical composition of Mo1−xWxS2 is demonstrated. Image credit: John Cavin, Washington University in St. Louis.