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Although direct methanol fuel cell offers high energy use efficiency and low pollution emission, the lack of suitable electrode materials poses a great challenge to its commercial application. Herein, a facile and scalable approach is developed to fabricate a hybrid electrocatalyst consisting of strongly coupled worm‐shape Pt nanocrystals and nitrogen‐doped low‐defect graphene (N‐LDG) sheets. Interestingly, it is found that the formation of Pt nanoworms (NWs) is induced by the N atoms in the high‐quality carbon matrix, which also allows the integration of their respective structural advantages and leads to a strong synergetic coupling effect. As a result, the obtained Pt NW/N‐LDG catalyst exhibits an extremely high mass activity of 1283.1 mA mg⁻¹ toward methanol oxidation reaction, accompanied by reliable long‐term stability and good antipoisoning ability, which are dramatically enhanced as compared with …