The fabrication of CrAl coatings for Lead-Cooled Fast Reactor (LFR) cladding applications was explored using High Power Impulse Magnetron Sputtering (HiPIMS). This study focused on the preparation, characterization, and performance evaluation of CrAl coatings to enhance their mechanical properties and resistance to lead‑bismuth eutectic (LBE) corrosion. The microstructures and mechanical properties of the coatings were analyzed to determine the optimal parameters, and the results emphasized the effects of the pulse width and frequency (collectively define the duty cycle). The advantages of HiPIMS technology are explained in comparison with traditional direct current magnetron sputtering. Optimized HiPIMS-prepared CrAl coatings exhibited an adhesion strength of 52 N, a hardness of 14 GPa, and a wear rate of 7 × 10 −7 mm 3/(Nm), compared to 10 N, 6 GPa, and 2.95 × 10 −5 mm 3/(Nm) for DCMS-prepared samples, respectively—demonstrating a marked improvement in coating performance. The coatings with optimized deposition parameters exhibited excellent LBE corrosion resistance, with no infiltration or degradation observed after 525 h of exposure at 550 °C. These results illustrated that CrAl coating is a promising candidate for LFR cladding protective materials. Additionally, HiPIMS was proven to be an effective method for producing protective coatings with enhanced mechanical strength.