The activation performance of quenchedTi-28V-15Mn-10Cr alloy, surface modified by using ball-milling with 10 wt.% LaNi3.55Co0.75Mn0.4 Al0.3 alloys was investigated. Compared with the plain Ti-28V-15Mn-10Cr alloy, the activation performance of the composite sample was remarkably improved. It was revealed that there is a layer of LaNi3.55Co0.75Mn0.4Al0.3 nanoparticles with an average grain size about 30 nm, covered on the surface of the composite sample. These nanoparticles accelerate the dissociation and absorption of hydrogen and then act as a window for hydrogen to enter the alloy bulk, resulting in an improvement of activation of the alloy.