Combining aluminum and steel offers a promising solution for reducing structural weight and fuel consumption across various industries. Pulse in tungsten inert gas (TIG) weld brazing effectively suppresses interfacial brittle intermetallics and enhances joint strength by influencing pool stirring and heat input during aluminum-to-steel joining. However, optimizing the pulsed TIG weld brazing process is challenging due to its numerous welding parameters. This study established statistical models for Al/steel joint strength without reinforcement using response surface methodology (RSM) based on central composite design (CCD). The models’ adequacy and significance were verified through analysis of variance (ANOVA). The four welding parameters influence weld strength in the following descending order: pulse on time > base current > pulse current > pulse frequency. Additionally, interactions between pulse current and pulse frequency, and between pulse on time and base current, were observed. Numerical optimization using RSM determined the optimal pulsed GTA weld brazing parameters for aluminum and stainless steel. With these optimized parameters, the joint strength reached 155.73 MPa, and the intermetallic compound (IMC) thickness was reduced to 3.4 μm.