Storage technologies are progressively emerging as a key measure to accommodate high shares of intermittent renewables with a view to guarantee their effective integration towards a profound decarbonisation of existing energy systems. This study aims to evaluate to what extent electricity storage can contribute to a significant renewable penetration by absorbing otherwise-curtailed renewable surplus and quantitatively defines the associated costs. Under a Smart Energy System perspective, a variety of future scenarios are defined for the Italian case based on a progressively increasing renewable and storage capacity feeding an ever-larger electrified demand mostly made up of electric vehicles and, to some extent, heat pumps and power-to-gas/liquid technologies. Results are compared in terms of crucial environmental and techno-economic indicators and discussed with respect to storage operating parameters. The outcome of this analysis reveals the remarkable role of electricity storage in increasing system flexibility and reducing, in the range 24–44%, the renewable capacity required to meet a given sustainability target. Nonetheless, such achievements become feasible only under relatively low investment and operating costs, condition that excludes electrochemical storage solutions and privileges low-cost alternatives that at present, however, exist only at a pilot or demonstration scale.