The heat treatment of a number of gas-atomised aluminium alloys prior to cold spraying recently showed that the resultant microstructural modification was accompanied by an improvement in deposition; however, the relationship between the microstructural homogenisation occurring after recrystallisation and the increase in deposition efficiency and particle-particle bonding had not been investigated. In this study, Al 6061 gas-atomised feedstock powder, before and after solution heat treatment, was cold sprayed and these materials were characterised using electron backscatter diffraction and transmission electron microscopy. The solution heat-treated Al 6061 powder showed large stress-free grains as opposed to the as-atomised feedstock powder which exhibited smaller grains with the presence of dislocations. The coating produced from as-received powder exhibited a homogeneous distribution of misorientation and lattice defects throughout the particles, whereas the coating produced from solution heat-treated powder showed a strain concentration in the interfacial zones. This was attributed to the partial dissolution and the clustering of solute atoms, allowing the aluminium matrix to deform around the newly formed precipitates.