Lower Cretaceous pedogenic carbonates exposed in SE China have been dated by U–Pb isotope measurements on single zircons taken from intercalated volcanic rocks, and the ages integrated with existing stratigraphy. δ13C values of calcretes range from –7.0‰ to –3.0‰ and can be grouped into five episodes of increasing–decreasing values. The carbon isotope proxy derived from these palaeosol carbonates suggests pCO2 mostly in the range 1000–2000 parts per million by volume (ppmV) at S(z) (CO2 contributed by soil respiration) = 2500 ppmV and 25°C during the Hauterivian–Albian interval (c. 30 Ma duration). Such atmospheric CO2 levels are 4–8 times pre-industrial values, almost double those estimated by geochemical modelling and much higher than those established from stomatal indices in fossil plants. Rapid rises in pCO2 are identified for early Hauterivian, middle Barremian, late Aptian, early Albian and middle Albian time, and rapid falls for intervening periods. These episodic cyclic changes in pCO2 are not attributed to local tectonism and volcanism but rather to global changes. The relationship between reconstructed pCO2 and the development of large igneous provinces (LIPs) remains unclear, although large-scale extrusion of basalt may well be responsible for relatively high atmospheric levels of this greenhouse gas. Suggested levels of relatively low pCO2 correspond in timing to intervals of regional to global enrichment of marine carbon in sediments and negative carbon isotope (δ13C) excursions characteristic of the oceanic anoxic events OAE1a (Selli Event), Kilian and Paquier events (constituting part of the OAE 1b cluster) and OAE1d. Short-term episodes of high pCO2 coincide with negligible carbon isotope excursions associated with the Faraoni Event and the Jacob Event. Given that episodes of regional organic carbon burial would draw down CO2 and negative δ13C excursions indicate the addition of isotopically light carbon to the ocean–atmosphere system, controls on the carbon cycle in controlling pCO2 during Early Cretaceous time were clearly complex and made more so by atmospheric composition also being affected by changes in silicate weathering intensity.