Carbon dioxide removal and solar radiation modification (SRM) are two classes of proposed climate intervention methods. A thorough understanding of climate system response to these methods calls for a good understanding of the carbon cycle response. In this study, we used an Earth system model to examine the response of global climate and carbon cycle to artificial ocean alkalinization (AOA), a method of CO2 removal, and reduction in solar irradiance that represents the overall effect of solar radiation modification. In our simulations, AOA is applied uniformly over the global ice-free ocean under the RCP8.5 scenario to bring down atmospheric CO2 to the level of RCP4.5, and SRM is applied uniformly over the globe under the RCP8.5 scenario to bring down global mean surface temperature to the level of RCP4.5. Our simulations show that with the same goal of temperature stabilization, AOA and SRM cause fundamentally different perturbations of the ocean and land carbon cycle. By the end of the 21st century, relative to the simulation of RCP8.5, AOA-induced changes in ocean carbonate chemistry enhances global oceanic CO2 uptake by 983 PgC and increases global mean surface ocean pH by 0.42. Meanwhile, AOA reduces land CO2 uptake by 79 PgC and reduces atmospheric CO2 concentration by 426 × 10−6. By contrast, relative to the simulation of RCP8.5, SRM has a minor effect on the oceanic CO2 uptake and ocean acidification. SRM-induced cooling enhances land CO2 uptake by 140 PgC and reduces atmospheric CO2 concentration by 63 × 10−6. A sudden termination of SRM causes a rate of temperature change that is much larger than that of RCP8.5. A sudden termination of AOA causes a rate of temperature change that is comparable to that of RCP8.5 and a rate of ocean acidification that is much larger than that of RCP8.5.