In the present work, the influence of solution viscosity on growth kinetics and purification efficiency in layer melt crystallization was investigated. Melt crystallization experiments were conducted for three different types of aqueous sucrose solution as they are ideal solutions and a relatively wide viscosity range can be investigated with a moderate change of freezing points. The aqueous 10 wt%, 23 wt%, and 30 wt% sucrose solutions have a dynamic viscosity value of 2.01 mPas, 4.74 mPas, and 7.21 mPas at their respective freezing points of −0.63 °C, −1.78 °C, and −2.64 °C. The solution temperature distribution was predicted by computational fluid dynamics (CFD) simulations run in COMSOL Multiphysics 5.6 software. Experimental results showed that a higher solution viscosity caused a higher crystal layer impurity and lower crystal yields in static layer melt crystallization. The cooling process of different solutions predicted by a CFD heat transfer study showed that the supersaturation region is wider for less concentrated solutions as cooling proceeds more rapidly. Hence, the temperature gradients obtained follow the boundary layer theory, i.e., the thinner the boundary layer, the faster the heat transfer.