Thermodynamic immiscibility is a challenge for intermetallic alloying of sub-5 nm Ru-based alloys, which are excellent electrochemical catalysts for water splitting. In this study, nanosecond laser ultrafast confined alloying (LUCA) is proposed to break the immiscible-to-miscible transition limit in the synthesis of carbon nanotubes (CNTs) supported sub-5 nm bimetallic RuM (M = Cu, Rh, and Pd) alloy nanoparticles (NPs). The alloying of non-noble metal Cu with varying atomic ratios of RuCu alloys is appealing owing to the low price of Cu and cost-effective synthesis for large-scale practical applications. Benefiting from the synergistic alloying effect and resultant H/OH binding energy alteration, the Ru