Extant models of long-term ecosystem nutrient status, largely formulated using data from mid- and low-latitude settings dominated by vascular vegetation, predict nitrogen (N) limitation in the early stages of primary succession and phosphorus (P) limitation in the latter stages. The aims of this study were a) to examine the use of mosses to establish ecosystem nutrient status; b) to test an existing model of nutrient limitation during long-term primary succession and c) to assess the connection between nutrient dynamics and the emergence of spatially structured vegetation in a high-latitude, moss-dominated community. Spatiotemporal changes in nutrient availability were inferred using tissue nutrient concentrations in a moss sampled from a long (850-year) chronosequence of lava flows in Iceland. This is the first use of bryophyte nutrient concentrations, even though they should be a good indicator of nutrient status in high-latitude habitats. Samples of the moss, Racomitrium lanuginosum, from different topographic positions were collected from seven lava flows of different ages (26–848 years) and analyzed to establish concentrations of N, P and major mineral nutrients. Concentrations of N were low on all sites and evidence of progressive N accumulation is lacking; increasing concentrations of phosphorus indicated increasing N limitation with terrain age. This pattern contrasts with other studies of long-term nutrient limitation, where N limitation reduces and P limitation increases with increasing terrain age. Concentrations of mineral nutrients did not vary significantly with terrain age. Nutrient concentrations were only weakly related to spatial patterning in the vegetation. It is likely that element concentrations were strongly influenced by inputs of allochthonous sediment. These findings suggest that mat-forming, pleurocarpous mosses may be used to infer long-term changes in N & P limitation during primary succession and that existing models of nutrient limitation may not be robust over century – millennial timescales in low productivity, high-latitude habitats.