Based on computational fluid dynamics (CFD), gas−liquid mass transfer in upward Taylor flow through vertical circular capillaries was studied. To save computational resources and time, the numerical simulations were carried out in a moving frame of reference attached to Taylor bubbles. Three consecutive Taylor bubbles were used to mimic the behavior of Taylor flow in an infinitely long capillary. Steady-state solutions of concentration fields were obtained to describe gas transfer from Taylor bubbles to the liquid phase. The liquid-phase volumetric mass-transfer coefficient, KLa, was investigated as a function of various parameters, including the liquid-film length, liquid-slug length, liquid-film thickness, bubble rise velocity, liquid-phase diffusivity, capillary diameter, and gravity. One fitted equation, expressed with three dimensionless numbers, was developed to quantify the relationship between KLa and the above parameters. The examples show that the equation could predict KLa well. The contributions of the cylindrical bodies and hemispherical caps of Taylor bubbles on the overall mass transfer were studied separately.