It is highly desirable to develop an energy generation system comprising a low-cost and earth-abundant non-noble metal catalyst for bifunctional electrocatalysis with good overall process performance, especially for applications in fuel cells or metal-air batteries. In this report, we show that nickel cobalt phosphite (NiCoÀ Phi) decorated with carbon nanotubes (CNTs) can perform as a bifunctional electrocatalyst for the oxygen evolution and oxygen reduction reactions (OER and ORR, respectively). The NiCoÀ Phi/CNT composite is synthesized by employing a simple, single-step hydrothermal method. The morphology of the composite consists of nanorod bundles of NiCoÀ Phi decorated with CNTs. The synthesized NiCoÀ Phi/CNT composite exhibits enhanced electrochemical OER activity with an overpotential of 400 mV at a current density of 10 mA/cm 2 and a Tafel slope value of 117 mV dec À 1 in 1 M KOH, possessing high stability towards the OER for 20 h. The ORR using the same catalyst shows an onset potential of 0.75 V and a Tafel slope of 100 mV dec À 1 in 0.1 M KOH with high-yield production of H 2 O 2 (85 %). The predominant formation of H 2 O 2 occurs mainly through a two-electron transfer process, as established by mass-controlled kinetic studies and has not been observed previously in these phosphorous oxy anion-based materials. The superior bifunctional nature of NiCoÀ Phi/CNT towards the OER and ORR arises from the synergistic effect of doped metal phosphites and CNTs.