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Interannual variability of air-sea CO2 exchange is an important metric that represents the interaction between the carbon cycle and climate change. Although previous studies report a large bias in the CO2 flux interannual variability in many Earth system models (ESMs), the reason for this bias remains unclear. In this study, the performance of ESMs in phase 5 of the Coupled Model Intercomparison Project (CMIP5) is assessed in the context of the variability of air-sea CO2 flux over the tropical Pacific related to El Nino-Southern Oscillation (ENSO) using an emission-driven historical experiment. Using empirical orthogonal function (EOF) analysis, the first principal component of air-sea CO2 flux shows a significant relationship with the Nino-3.4 index in both the observation-based product and models. In the observation-based product, the spatial pattern of EOF1 shows negative anomalies in the central Pacific, which is, however, in contrast to those in several ESMs, and even opposite in sign to those in HadGEM2-ES and MPI-ESM-LR. The unrealistic response of the air-sea CO2 flux to ENSO mainly originates from the biases in the anomalous surface-water CO2 partial pressure (). A linear Taylor expansion by decomposing the anomalous into contributions from salinity, sea surface temperature, dissolved inorganic carbon (DIC), and alkalinity is applied to diagnose the biases. The results show that decreased during El Nino results from reduced upwelling of high-concentration DIC from deeper layers that overwhelms the increasing caused by warmer sea surface temperature. Overly weak reduction of vertical motion during El Nino and weak vertical gradients of climatological DIC concentration are the main reasons for biases in the negative surface DIC anomalies and eventually the anomalies. This study highlights the importance of both physical ocean responses to El Nino and climatological distributions of carbon-related tracers in the simulation of the interannual variability of air-sea CO2 fluxes.