The rational fabrication of highly efficient electrocatalysts with low cost toward oxygen evolution reaction (OER) is greatly desired but remains a formidable challenge. In this work, we present a facile and straightforward method of incorporating NiCo-layered double hydroxide (NiCo-LDH) into GO-dispersed CNTs (GO-CNTs) with interconnected configuration. X-ray absorption spectroscopy (XAS) reveals the strong electron interaction between NiCo-LDH and the underlying GO-CNTs substrate, which is supposed to facilitate charge transfer and accelerate the kinetics for OER. By tuning the amount of CNTs, the optimized NiCo-LDH/GO-CNTs composite can achieve a low overpotential of 290 mV at 10 mA·cm⁻² current density, a small Tafel slope of 66.8 mV·dec⁻¹ and robust stability, superior to the pure NiCo-LDH and commercial RuO₂ in alkaline media. The preeminent oxygen evolution performance is attributed to the synergistic effect stemming from the merits and the intimate electron interaction between LDH and GO-CNTs. This allows NiCo-LDH/GO-CNTs to be potentially applied in an industrial non-noble metal-based water electrolyzer as the anodic catalysts.