An alternative electrodeposition method was introduced for TiB2 growth. Ti and B were co-deposited from the environmentally friendly electrolyte to form TiB2. A compact, 40 μm thick TiB2 layer was grown after 240 min at 850 °C and 70 mA/cm2. The grown TiB2 has the hardness value as high as 3000 ± 200 HV. The diffusion zone (DZ) formation was seen with the hardness of 1000 ± 100 HV.