We present new geochemical, Sm–Nd and U–Pb data on the felsic volcanic rocks containing the world-class volcanic-hosted massive sulphide deposits in the Riotinto–Nerva unit, Iberian Pyrite Belt, Spain. Three new U–Pb ages from older plagioclase–quartz-phyric dacites and plagioclase-phyric rhyolites to youngest plagioclase–quartz-phyric rhyolites indicate a time span for felsic volcanism ranging from 351.5 ± 0.4 to 345.7 ± 0.6 Ma. The youngest felsic rocks exhibit lower ε _Nd , as well as contrasting Ti, Sr, Zr, Hf and Eu/Eu* values. We interpret that in the Riotinto–Nerva unit crustal melting successively affected shallower, more evolved horizons in the crust. Progressive crustal melting is consistent with current interpretations of the Iberian Pyrite Belt in terms of a late Devonian–Early Carboniferous transtensional setting, coupled with underplating by basic magma. We suggest that low ε _Nd , evolved crustal magmatism could be used as a proxy in studies of the genesis of these and possibly other Phanerozoic massive sulphide deposits. Supplementary material: Details of the analytical methods and whole-rock data for basalts are available at http://www.geolsoc.org.uk/SUP18452 .