Following major disturbances ecosystem development occurs but in the prolonged absence of disturbance a decline (retrogressive) phase follows in which productivity and nutrient availability diminishes. Although it is recognized that litter quality and decomposition rates decrease as retrogression proceeds, little is known about the extent to which this is driven among- vs. within-species variation across these sequences. 2. We selected six long-term chronosequences that each included retrogressive stages, in New Zealand, Hawaii, Sweden, Alaska and Australia. Two involve significant species turnover across the sequence so that different species dominate at different stages, two involve low species turnover so that the same dominant species occur at all stages, and two involve some turnover of species but with certain species persisting throughout most of the sequence. 3. For each chronosequence, we collected litter from each dominant plant species at each stage of that sequence. For each litter collection we measured concentrations of N and P, and performed laboratory decomposition bioassays to measure mass loss, N and P loss, and the response of mass loss to mixture with litters of coexisting species. 4. We found that litter N and P concentrations often declined with increasing ecosystem age, both among- and within-species. However, the relative importance of among- and within-species effects varied across the six chronosequences. Rates of litter mass, N, and P loss during decomposition sometimes decreased with increasing ecosystem age, but most often at the among-species rather than the within-species level. 5. Litter mixing effects often varied across chronosequence stages, but the magnitude and direction of these effects was inconsistent among sequences. Variation in litter mixing effects across chronosequence stages was driven mainly by among- rather than within-species variation. 6. Although several recent studies have emphasized the role of within-species variation on ecosystem properties, our results point to among-species variation as a consistently important ecological driver, with within-species variation being important only for some variables and in some instances. As such they highlight that decomposition processes are most likely to be highly responsive to gradients of soil fertility (such as across chronosequences) when significant species turnover occurs across the gradient. © 2008 British Ecological Society.