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Development of efficient and cost‐effective transition metal‐based catalysts for overall water splitting is desired. Herein, a facile synthesis procedure for the development of FeCo bimetallic alloy nanoparticles (NPs) located on the tips of multi‐walled carbon nanotubes (CNTs) supported over N‐doped carbon nanofibers (CNFs) is presented. The CNTs, not only prevent FeCo NPs from agglomeration by encapsulating them at the tip but also provide an efficient electron pathway. The materials exhibited excellent performance in oxygen evolution reaction (OER) and decent activity in hydrogen evolution reaction (HER) with long‐term durability of up to 48 hours on glassy carbon electrode. The best OER activity with a overpotential of 283 mV@10 mAcm−2 and Tafel slope of 38 mV/dec was achieved with a hierarchically porous catalyst having Fe : Co molar ratio of 1 : 2. This synthesis approach is promising for growing well‐dispersed CNTs over N‐doped carbonaceous support using bimetallic alloys for electrocatalytic applications. [ABSTRACT FROM AUTHOR]