In conclusion, we explored a new type of layered heterostructures, frustrated van der Waals heterostructures (Fvd-WHs). A FvdWH is a layered material with alternating strains and compressions, where one layer is strained and the adjacent layer is compressed. Using density functional theory with the r 2 SCAN+rVV10 exchange-correlation potential, we explored the stability of 9 FvdWHs that are made from dynamically stable monolayers, and found 8 FvdWHs that are more thermodynamically stable with alternating strains and compressions than the corresponding material without any strains. Two of these materials were found to be maintain their structures after ab initio molecular dynamics simulations at 300 K. We presented a scheme for the potential stacking of strained/compressed 2D materials to build FvdWHs, and expect this class of materials to harbour novel physical and chemical phenomena.