Coupled climate model simulations of volcanic eruptions and abrupt changes in CO2 concentration are compared in multiple realizations of the Geophysical Fluid Dynamics Laboratory Climate Model, version 2.1 (GFDL CM2.1). The change in global-mean surface temperature (GMST) is analyzed to determine whether a fast component of the climate sensitivity of relevance to the transient climate response (TCR; defined with the 1%yr-1 CO2-increase scenario) can be estimated from shorter-time-scale climate changes. The fast component of the climate sensitivity estimated from the response of the climate model to volcanic forcing is similar to that of the simulations forced by abrupt CO2 changes but is 5%-15% smaller than the TCR. In addition, the partition between the top-of-atmosphere radiative restoring and ocean heat uptake is similar across radiative forcing agents. The possible asymmetry between warming and cooling climate perturbations, which may affect the utility of volcanic eruptions for estimating the TCR, is assessed by comparing simulations of abrupt CO2 doubling to abrupt CO2 halving. There is slightly less (~5%) GMST change in 0.5 × CO2 simulations than in 2 × CO2 simulations on the short (~10 yr) time scales relevant to the fast component of the volcanic signal. However, inferring the TCR from volcanic eruptions is more sensitive to uncertainties from internal climate variability and the estimation procedure. The response of the GMST to volcanic eruptions is similar in GFDL CM2.1 and GFDL Climate Model, version 3 (CM3), even though the latter has a higher TCR associated with a multidecadal time scale in its response. This is consistent with the expectation that the fast component of the climate sensitivity inferred from volcanic eruptions is a lower bound for the TCR.