Improving the pseudocapacitance performance of layered double hydroxides (LDH) based catalysts is critical for enhancing energy density in electrochemical storage applications, such as supercapacitance and batteries. This study examines the effect of decoration with Ni, Co, and NiCo nanocomposites (NCs) on the pseudocapacitance performance of NiCo LDH nanoflowers. The NiCo LDH nanoflowers are electrodeposited using the cyclic voltammetry technique, while metal decoration is performed using the cathodic chronoamperometry technique. A clear dependence on the decorated transition metal type is observed in the surface morphology, chemical bonding states, and corresponding pseudocapacitance performance. The decoration of NiCo LDH nanoflowers with excess transition metals of the same kind, Ni and Co, strongly enhances electron coupling and charge transfer kinetics. The hybrid NiCo@NiCo LDH nanoflowers exhibit better pseudocapacitance performance than those decorated with only Ni or Co. The hybrid NiCo@NiCo LDH nanoflowers demonstrate the highest specific capacitance (C_sp) of 2110 mF∙cm^–2 (211 mA∙cm^–2) at 1 mA∙cm^–2 and retain 86 % of their C_sp at 10 mA∙cm^–2. The assembled asymmetric supercapacitor of NiCo@NiCo LDH || activated carbon reveals high energy density (E) of 145.1 μWh∙cm^–2 at a powder density (P) of 5.12 mW∙cm^–2, keeping a high E of 75 μWh∙cm^–2 at a higher P of 51.92 mW∙cm^–2.