Al-based fully amorphous coatings with low porosity were successfully produced via warm spraying, combining numerical simulation and experimental validation. A warm spray gun model, employing computational fluid dynamics, was developed to simulate the warm spraying process. The study delved into the effects of reactant flow rate, oxygen/fuel (O/F) ratio, coolant flow rate, spray distance, particle size, particle shape, particle injection velocity, and particle injection angle on the gas flow field parameters (pressure, temperature, and velocity) and particle in-flight behaviors (temperature, velocity, and in-flight trajectory). The optimum spraying parameters (OSP) predicted by the simulation results were determined: 0.008740 kg/s for reactant flow rate, 2.7 for the O/F ratio, 0.007356 kg/s for coolant flow rate, 142 mm for spraying distance, 10–35 μm for particle size range, spherical for particle shape, 10 m/s for particle injection velocity, and 0° for particle injection angle. Subsequently, warm spraying experiments based on the OSP yielded Al-based fully amorphous coatings with a porosity of 0.08 %. This work provides valuable insights for the production of Al-based fully amorphous coatings with minimal porosity through warm spraying.