Spray dry scrubbing is widely used for SO2 abatement, but high removal efficiencies are required for economical operation. Whereas SO2 removal dependence on the drying rate has been investigated, available modelling work has not addressed the impact of selected drying models on the removal efficiency; instead, a single drying model is often assumed. In the present work, computational fluid dynamics is used to numerically model the SO2 removal in a laboratory-scale spray dry scrubber. The Euler–Lagrangian framework is used to simulate the multiphase interaction and two drying models are used: the widely used classical D2-law model and the mechanistic model. In addressing shortcomings from previous works, this study also provides a comprehensive model development and robust model validation with quantifiable metrics for goodness-of-fit, including R2. Also presented are key parameters associated with SO2-removal efficiency, including the exit product moisture content and droplet dynamics. The mechanistic model gave a better representation of the SO2-removal efficiency. The latter was found to be dependent on the inlet temperature, the calcium-to-sulphur and liquid-to-gas (L/G) ratios, with a high L/G ratio having the most significant impact on the removal efficiency, although resulting in a higher product outlet moisture content.