Hydrogen (H2) is a valuable, cleanly combustible, and high-energy fuel, and catalytic methanol steam reforming (MSR) is a possible scale-up method to increase H2 production. We propose a new Ni-MOF-derived carbon (MDC) catalyst synthesized by pyrolyzing a Ni-BTC structure to conduct this reaction due to its high dispersion and strong metal-support interaction (SMSI), aiming towards lower metal consumption and higher performance and stability. Through extensive characterization, two sizes of Ni particles were discovered on the surface: 1) large and loosely bound particles (14.26 nm), and 2) fine particles (8.77 nm). After exposing the Ni-BTC structure to aqua regia (Ni-MDC (AR)), the larger Ni particles were removed, while the finer particles remained due to the SMSI. Within a fixed-bed reactor operating at atmospheric pressure, both MDC catalysts showed similarly high MSR catalytic activity (∼90–100% conversion and ∼70% H2 selectivity at 600–700 °C), which indicates the presence of a strong nickel-carbon interface caused by the finer particles, even though this also resulted in slow initial activation and fast subsequent deactivation, especially after acid treatment, thereby requiring further research to improve upon this.