The shift in ecosystem multifunctionality during ecosystem succession (years to decades) remains largely unexplored. In this study, we used a 120-year-old pine temperate forest chronosequence (1: 1–19 years, stage 2: 20–39 years, stage 3: 40–59 years, stage 4: 60–79 years, stage 5: 80–99 years, stage 6: 100–120 years) to evaluate the role that time plays in shaping ecosystem multifunctionality (nutrient cycling, carbon stocks, water regulation, decomposition and wood production), and found that, over the first century, ecosystem functioning gradually increased every ~50 years. Such a result was maintained for individual groups of ecosystem functions and services including nutrient cycling, carbon stocks, decomposition and wood production. Plant diversity and soil stoichiometry (C:N ratio) were the major environmental predictors for the changes in ecosystem multifunctionality during forest secondary succession. Plant diversity increased during ecosystem succession and was positively related to ecosystem multifunctionality. The soil C:N ratio decreased during ecosystem succession and was negatively related to multifunctionality. Our results suggest that increases in aboveground resource heterogeneity (higher plant diversity) and organic matter quality (lower soil C:N ratios) could help explain the increases in multifunctionality over a century of forest development. Our work illustrates the importance of time in shaping multifunctionality during the first century of ecosystem succession, and further provide important insights for the management of temperate forest ecosystems.