Long-duration energy storage is commonly viewed as a key technology for providing flexibility to the grid and broader energy systems over a multidecadal time frame. However, prior work has typically used present-day grid infrastructures to characterize the relationship between the duration and arbitrage value of storage in electricity markets. This study leverages established National Renewable Energy Laboratory grid planning and operations tools, analysis, and data to execute a price-taker model of an energy storage system for several 8760 h price series representative of current and future contiguous United States grid infrastructures with varying shares of variable renewable energy (VRE). We find that the total value of energy storage typically increases with VRE shares, but any increase in the relative value of longer storage durations over time depends on the region and grid mix. Some regions see incremental value increasing notably, up to 20–40 h in 2050, while others do not. The negative effect of lower roundtrip efficiency on value is also found to be scenario-dependent, with the energy value in higher VRE scenarios being less sensitive to roundtrip efficiency and more supportive of longer storage durations. Long-duration storage value and deployment potential are a function of evolving electricity sector infrastructure, markets, and policy, making it critical to consistently revisit potential long-duration storage contributions to the grid.