This work presents a systematic study to synthesize NiO on nickel foam (NF) using a straightforward and cost‐efficient hydrothermal method, followed by calcination. Through comprehensive physicochemical analyses, it was demonstrated that the properties of the resultant NF@NiO could be modulated by adjusting the concentration of the nickel nitrate hexahydrate precursor. Notably, a morphological transition from a 2D sheet‐like structure to a 3D rambutan‐like formation was observed as the precursor concentration increased. The best‐performing NF@NiO 4 mM showed a maximum areal capacity of 723 mC cm‐2 (equivalent to 547.73 F g‐1) at a current density of 0.5 mA cm‐2. This electrode also maintained remarkable cycle stability, retaining 78.9% of its capacitance after 10,000 cycles at a current density of 50 mA cm‐2 in 2 M KOH. Furthermore, ASC (NiO 4 mM//AC) achieved a specific capacitance of 64.79 F g‐1 at a current density of 1 A g‐1 with an energy density of 17.63 Wh kg‐1 at a power density of 700 W kg‐1.