The work aims to adjust the microstructure of cold-sprayed Ni-Al coating, enhance the contact area of coating elements and improve the reaction velocity of coating. The cast steel pills were added into the mixed powder of Ni and Al to study the influence of in-situ shot peening on the microstructure, mechanical property and reaction characteristics of Ni-Al coating. The microstructure and contact area between Ni and Al were characterized by scanning electron microscopy (SEM) and quantitative metallography analysis. The compressive mechanical properties of Ni-Al coating were measured by the universal material testing machine and split Hopkinson bar (SHPB). The reaction temperature and heat release of Ni-Al coating were tested by differential scanning calorimetry (DSC). The self-propagating reaction process and combustion speed of Ni-Al coating were analyzed by high-speed cameras. The Ni-Al energetic structural coating deposited by in-situ shot peening assisted cold spraying was dense and free from macro cracks. The shot peening effect enhanced the deformation extent of the Ni particles inside the coating and contact area between Ni and Al phases significantly while having no obvious effect on the density and composition of Ni-Al coating. The static and dynamic compression strengths of Ni-Al coating deposited by in-situ shot peening assisted cold spraying were 210~250 MPa and 310~335 MPa, separately. The reaction activity was enhanced and the reaction start temperature decreased to 422 ℃ with the addition of shot peening pills and the self-propagating combustion speed of Ni-Al energetic structural coating was significantly increased. As the volume of pills was 77%, the combustion speed of Ni-Al coating reached 416 mm/s, which was about five times that of Ni-Al coating without addition of cast steel pills. The in-situ shot peening assisted cold spraying can enhance the activity of cold-sprayed Ni-Al energetic structural coating without the loss of mechanical property. The combustion speed of Ni-Al coating can be enhanced significantly, while the content of shot peening pills has no obvious effect on the content of coating.