The grain structure evolution and nanomechanical behavior of cold-sprayed Al coating on Ti substrate with friction stir spot processing (FSSP) were studied by the electron backscatter diffraction and nanoindentation methods. The low-angle boundaries (LAGBs) fraction and the density of the geometrically necessary dislocations (GNDs) decreased from the base zone (BZ) to the stir zone (SZ). The average grain size, the LAGBs fraction and the density of the GNDs were various in different locations of the SZ, which can be attributed to the variety of local shear strain and temperature gradient during FSSP. The B/\(\stackrel{{-}}{\text{B}}\) component, the C component, and the A*1/ A*2 component were mainly developed in the SZ. The highest intensity of the B/\(\stackrel{{-}}{\text{B}}\) component appeared in the 3/8D of the SZ, indicating that the plasticized materials flowed downward experienced the highest shear strain. The materials in the heat affected zone (HAZ) underwent static recrystallization, while the continuous dynamic recrystallization (CDRX) and the geometric dynamic recrystallization (GDRX) occurred in the thermo-mechanically affected zone (TMAZ) and SZ. The nano-hardness and elastic modulus of the cold-sprayed Al coating after FSSP were comparable to those of pure Al bulk. The grain size and dislocation density were the main factors affecting the nano-hardness in the SZ.