Formic acid (FA, HCOOH), a convenient and safe hydrogen storage material, has the great potential for fuel cell applications. However, hydrogen generation of FA is inefficient in the presence of heterogeneous catalysts at relatively low temperatures, which remains a big challenge. Herein, La2O3-modified highly dispersed AuPd alloy nanoparticles (AuPdLa2O3) with small particle size have been successfully anchored on carbon nanotubes (CNTs) by a facile co-reduction route. Moreover, the catalyst exhibits excellent catalytic activity and 100% hydrogen selectivity for hydrogen generation in the formic acid/sodium formate (FA/SF) system with the initial turnover frequency (TOF) value of 589 mol H2 mol−1 catalyst h−1 at 50 °C and 280 mol H2 mol−1 catalyst h−1 even at room temperature (25 °C). The present Au0.3Pd0.7-(La2O3)0.6/CNTs with superior catalysis on FA dehydrogenation without any CO generation at room temperature can not only pave the way for practical application of hydrogen storage system, but also can be extended to other catalysis system.