This work presents a study on the fabrication of polymethyl methacrylate (PMMA) coatings on NiTi alloys using the spin-coating technique, combining numerical simulation with COMSOL Multiphysics 6.3 and experimental validation. This study provides a numerical framework and parametric study of a COMSOL-based simulation framework for estimating the PMMA coating thickness during the spin-coating process. We present an axisymmetric numerical framework, consistent with classical analytical trends; we provide parametric maps (viscosity, rpm, volume) to delimit thickness ranges (e.g., 100–300 μm). Limitations with no experimental validation are included and evaporation is not modeled; therefore, the figures are indicative estimates. The spin-coating parameters, such as the rotation speed, internal pressure, viscosity of the PMMA solution, and initial volume of the polymer solution, are considered important factors for the simulation process. The coating parameters determine the thickness of the coating layer achieved during the process of spin coating. The 2D axisymmetric flow considers internal factors of a surface tension of 0.07 N·m, a contact angle of 90°, and a density of 1150 kg/m3 for the coating process without evaporation effects. The moving mesh (coating layer) is considered a free surface without any slip boundary with the substrate surface. The coating thickness was determined by various rotations and dynamic viscosities, using a simulation method. The experimental findings and simulation output of the coating thickness as a function of various dynamic viscosities and rotations match well. The final coating thickness ranged from 100 to 300 μm, depending on a viscosity of 11 mPa·s and 100, 500 rpm.