Ecosystem functioning depends on biodiversity at multiple trophic levels, yet relationships between multitrophic diversity and ecosystem multifunctionality have been poorly explored, with studies often focusing on individual trophic levels and functions and on specific ecosystem types. Here, we show that plant diversity can affect ecosystem functioning both directly and by affecting other trophic levels. Using data on 13 trophic groups and 13 ecosystem functions from two large biodiversity experiments—one representing temperate grasslands and the other subtropical forests—we found that plant diversity increases multifunctionality through elevated multitrophic diversity. Across both experiments, the association between multitrophic diversity and multifunctionality was stronger than the relationship between the diversity of individual trophic groups and multifunctionality. Our results also suggest that the role of multitrophic diversity is greater in forests than in grasslands. These findings imply that, to promote sustained ecosystem multifunctionality, conservation planning must consider the diversity of both plants and higher trophic levels.