Cataphoresis varnishing enables an organic coating to form on an aluminum substrate, thus increasing its corrosion resistance and durability. Cataphoresis varnishing is known to ensure a high adhesion of the created cataphoresis layer and a good homogeneity of this layer, even on surfaces with complex geometry. This paper aimed to optimize the deposition process and to analyze and evaluate the thickness of a cataphoresis layer formed on an aluminum substrate from AW 1050—H24 material. In total, 30 separate samples were created in accordance with the Design of Experiments methodology, using a central composite plan. The independent input factors in the study were: the electrical voltage (U) and deposition time in the cataphoresis varnishing process (tKTL) at the polymerization times of 15 min, 20 min, and 25 min, respectively. The results of the statistical analysis showed that the voltage accounted for 33.82% of the change in the thickness of the created layer and the deposition time contributed 28.67% to thi change. At the same time, the interaction of the voltage and deposition time (p < 0.0001) accounted for 20.25% of the change in the thickness of the layer under formation. The regression model that was constructed showed a high degree of prediction accuracy (85.8775%) and its use as a function for nonlinear optimization provided a maximum layer thickness th of max = 26.114 µm, at U = 240 V and tKTL = 6.0 min, as was proven under experimental conditions.