Studies of storage and production of hydrogen, which is an alternative to fossil fuels, have been intensified. Hydrogen production from metal borohydrides via catalyst is very attractive because of its advantages, such as controlled production, high hydrogen content, nontoxicity, etc. In this study, the catalytic performances of nanoporous nickel−chromium alloy and nickel−vanadium alloy catalysts prepared with magnetron sputtering in hydrolysis of potassium borohydride, which is a hydrogen storage material, were investigated. Parameters that affected the hydrolysis reaction rate, such as the temperature, the amount of catalyst, and the volume of 0.5 M HCl solution were investigated using response surface methodology. In addition, the prepared catalysts were characterized with XRD and FE-SEM analysis, and the remaining solutions after the reactions were characterized with FE-SEM/EDS analysis. Using response surface methodology, optimum conditions for the maximum hydrogen production rate were determined to be 1.65 g of catalyst, 6% KBH4, 3% NaOH, and 7 mL of 0.5 M HCl at 333 K. Under these conditions, the hydrogen production rates were calculated as 68.9 L·min−1·gcat−1 and 76.5 L·min−1·gcat−1 for NiCr and NiV, respectively.