Fourth-generation nuclear power systems are based on high-temperature gas-cooled reactors, in which the pebble fuel is the primary energy carrier. In this regard, applying protective pyrocarbon coatings on granulated fuel is an essential problem in ensuring the reliability of nuclear power plants. The article’s main idea is to research rational technological parameters of forming a pyrocarbon protective coating on the granules of a nuclear fuel model. For this purpose, granulated Al2O3 with the protective pyrocarbone coating was applied as a fuel model. The article’s aim is to study the effect of thermophysical parameters on applying a protective pyrocarbon coating on granulated Al2O3. During the experimental studies, thermal imaging of the pyrolysis process was used. The scientific novelty of the work is the equilibrium curves for the systems Al2O3:CH4, Al2O3:CH4:N2, and Al2O3:CH4:Ar. Their analysis allowed for evaluating rational thermochemical parameters of the pyrolysis process. As a result, rational thermophysical parameters of coating granulated Al2O3 with a pyrocarbon layer were evaluated, and the practical possibility of applying the pyrocarbon coating to granulated Al2O3 in the electrothermal fluidized bed was experimentally proven. It was shown that nitrogen does not significantly affect the target reaction product under a temperature of less than 1500 K. Also, the rational conditions for the pyrocarbon coating at a pressure of 0.1 MPa were realized at a temperature of 900–1500 K and using argon. Moreover, pyrocarbon was precipitated from hydrocarbon at 1073–1273 K. Overall, the need to add an inert gas for reducing the carbon black formation was proven to prevent a reduction of natural gas efficiency.