This study presents lithium isotope and elemental data for the dissolved phase and suspended and bedload sediments of the major Icelandic rivers. For the dissolved phase, δ7Li values range between 10.1‰ and 23.8‰, while river sediments display lower and much more homogeneous values (δ7Li = 3.1‰–4.8‰), close to the composition of unweathered Mid-Ocean Ridge Basalt (MORB). High δ7Li values are associated with high K/Li, Na/Li and Mg/Li ratios, in waters draining mainly old and weathered basalt catchments, whereas low δ7Li rivers are located in younger parts of the island. Simple mixing between precipitation, Li-rich hydrothermal springs and basalt weathering is unable to explain the entire range of δ7Li values. Instead, a simple model of Li uptake by secondary minerals, associated with clay–water Li isotope fractionation (Δ7Li ranging from − 1‰ to - 7.5‰) can explain both water and sediment δ7Li values. A negative correlation is observed between basalt chemical erosion rates and δ7Li measured in Icelandic rivers, and an empirical law is inferred. Comparison with literature data suggests that this relationship may be applicable at a more global scale, and, if confirmed, could be of particular use for estimating the evolution of continental weathering preserved in marine sedimentary records. However, more data are now needed for rivers draining silicates typical of the continental crust, in order to refine large scale modelling.