Volcanoes are a key natural source of CO2, but global estimates of volcanic CO2 flux are predominantly based on measurements from a fraction of world's actively degassing volcanoes. We combine high‐precision airborne measurements from 2016 and 2017 with atmospheric dispersion modeling to quantify CO2 emissions from Katla, a major subglacial volcanic caldera in Iceland that last erupted 100 years ago but has been undergoing significant unrest in recent decades. Katla's sustained CO2 flux, 12–24 kt/d, is up to an order of magnitude greater than previous estimates of total CO2 release from Iceland's natural sources. Katla is one of the largest volcanic sources of CO2 on the planet, contributing up to 4% of global emissions from nonerupting volcanoes. Further measurements on subglacial volcanoes worldwide are urgently required to establish if Katla is exceptional, or if there is a significant previously unrecognized contribution to global CO2 emissions from natural sources.