Particle number concentration in the troposphere is an important parameter controlling the climate and health impacts of atmospheric aerosols. We show that nucleation rates and total particle number concentrations in the troposphere, predicted by different nucleation schemes, differ significantly. Our extensive comparisons of simulated results with land-, ship-, and aircraft-based measurements indicate that, among six widely used nucleation schemes involving sulfuric acid, only the ion-mediated nucleation (IMN) scheme can reasonably account for both absolute values (within a factor of ∼2) and spatial distributions of particle number concentrations in the whole troposphere. Binary homogeneous nucleation (BHN) schemes significantly underpredict particle number concentration in the lower troposphere (below ∼500 mbar), especially in the boundary layer over major continents (by a factor of up to ∼10). BHN is also insignificant in the upper troposphere based on a recent kinetically self-consistent nucleation model constrained by multiple independent laboratory data. Previous conclusions about the importance of BHN in the upper troposphere should be revisited. Empirical activation and kinetic nucleation formulas significantly overpredict the particle number concentrations over tropical and subtropical oceans (by a factor of up to ∼10 in the boundary layer), and the overpredictions extend from ocean surface to around ∼400 mbar. This study represents the first comprehensive comparison of global particle number simulations with relevant measurements that have a 3-D global spatial coverage. Our results suggest that ion-mediated H2SO4-H2O nucleation appears to dominate over neutral H2SO4-H2O nucleation, not only in the lower troposphere but also in the middle and upper troposphere.