Co–B/Chi, which is made up of highly distributed Co–B particles, was synthesized by impregnation and chemical reduction methods. Scanning electron microscopy, energy-dispersive spectroscopy, X-ray diffraction, Brunauer–Emmett–Teller adsorption and Fourier transform infrared spectroscopy analyses were used to describe the morphology and microstructure of Co–B/Chi. The synthesized catalyst showed high catalytic activity in the hydrolysis reaction of NaBH4. The unsupported Co–B samples were compared with the chitin-supported Co–B catalyst, and the result showed that higher catalytic activity and good cycling stability for NaBH4 hydrolysis were obtained with the chitin-supported catalyst. The reaction conditions were investigated to achieve high hydrogen production. The maximum rate of hydrogen production was obtained at 40 °C and 20 mg catalyst amount. At ideal conditions, the hydrolysis reaction’s activation energy was determined to be 51.65 kJ mol−1. It is indicate that Co–B/Chi is a viable low-cost catalyst for the hydrolysis of NaBH4 for hydrogen production.