Recently, hydrazine borane (HB, N2H4BH3) is recognized as an ideal chemical hydrogen storage material due to its high efficiency in storing hydrogen and excellent stability. However, finding an efficient, stable, and low-cost catalyst is still a challenge. In this study, CoPt nanoparticles (NPs) supported on carbon nanotubes (CNTs) are prepared at room temperature. The Co0.4Pt0.6/CNTs catalyst exhibits optimal catalytic performance for hydrogen production from HB at ambient conditions, achieving a total turnover frequency (TOF) value of 1525.4 h−1 and 100% H2 selectivity. The well-dispersed CoPt NPs on CNTs and the synergistic effect between Co and Pt further enhance the decomposition efficiency of HB. This high-performance catalyst has significant implications for the advancement of hydrogen storage materials, particularly in relation to HB.