The UK Countryside Survey (CS) is a national long-term survey of soils and vegetation that spans three decades (1978–2007). Past studies using CS data have identified clear contrasting trends in topsoil organic carbon (tSOC) concentrations (0–15 cm) related to differences between habitat types. Here we firstly examine changes in tSOC resulting from land use change, and secondly construct mixed models to describe the impact of indirect drivers where land use has been constant. Where it occurs, land use change is a strong driver of SOC change, with largest changes in tSOC for transitions involving SOC-rich soils in upland and bog systems. Afforestation did not always increase tSOC, and the effect of transitions involving woodland was dependent on the other vegetation type. The overall national spatial pattern of tSOC concentration where land use has been constant is most strongly related to vegetation type and topsoil pH, with contributions from climate variables, deposition and geology. Comparisons of models for tSOC across time periods suggest that declining SO4 deposition has allowed recovery of topsoils from acidification, but that this has not resulted in the increased decomposition rates and loss of tSOC which might be expected. As a result, the relationship between pH and tSOC in UK topsoils has changed significantly between 1978 and 2007. The contributions of other indirect drivers in the models suggest negative relationships to seasonal temperature metrics and positive relationships to seasonal precipitation at the dry end of the scale. The results suggest that the CS approach of long-term collection of co-located vegetation and soil biophysical data provides essential tools both for identifying trends in tSOC at national and habitat levels, and for identifying areas of risk or areas with opportunities for managing topsoil SOC and vegetation change.