Designing and developing highly active, stable, and cost-effective hydrogen evolution reaction (HER) catalysts is crucial in the field of water electrolysis. In this study, we utilize N-doped porous carbon (CoNC) derived from zeolite imidazole metal–organic frameworks (ZIF-67) as support and prepare CoNC-Pt-IM-P via chemical impregnation (CoNC-Pt-IM) and plasma treatment. Systematic analyses reveal that calcined CoNC with pyridinic nitrogen could serve as a robust support to strongly anchor PtCo nanoclusters, while argon plasma treatment could lead to a noticeable aggregation of Co and Pt atoms so as to alter the electronic environment and enhance intrinsic HER catalytic activity. CoNC-Pt-IM-P could exhibit outstanding catalytic activity toward HER, achieving an exceptionally low overpotential of 31 mV at the current density of −10 mA cm−2 and a Tafel slope of 36 mV dec−1. At an overpotential of 50 mV, its mass activity reaches 4.90 A mgPt−1, representing enhancements of 1.5 times compared to CoNC-Pt-IM and 12.3 times compared to commercial 20 wt% Pt/C. Furthermore, it could operate stably for over 110 h at a current density of −10 mA cm−2, demonstrating its exceptional durability. This work uses plasma treatment to achieve the controllable aggregation of Co and Pt atoms to enhance their catalytic activity, which has the advantage of avoiding excessive particle aggregation compared to the commonly used method of high-temperature calcination.