Crystallization fouling is a typical problem in heat exchangers, which leads to the deterioration of heat transfer performance and energy loss. Surface modification and fluid shear are important factors to control crystal nucleation, aggregation, growth, and removal. This study performed static fouling experiments of calcium sulfate crystallization on patterned polymethyl methacrylate for different stages and real-time dynamic fouling experiments on metal surfaces. The grooves provide nucleation sites, and the nuclei prefer aggregation, forming blossoming-like crystals. After washing the fouled sample with distilled water, the size of blossoming-like crystals decreases and it is difficult to fully clean blossoming-like crystals compared with dispersed crystals. The fouling performance for the second time after the cleaning demonstrates that the existent crystals create nucleation sites, leading to a higher deposition rate than that of the first fouling. Furthermore, the fouling morphology is flaky gypsum on the metal surfaces under the dynamic experiment and fouling removal caused by the fluid shear is obvious. The deposition mass per unit area on metal materials under dynamic experiment in descending order is 0.0353 mg/mm2 of copper, 0.0154 mg/mm2 of titanium, 0.0146 mg/mm2 of aluminum, and 0.0070 mg/mm2 of stainless steel, respectively, which is significant to the mitigation of crystallization fouling on different materials.