Cold spray (CS) is an emerging technology for repairing and 3D additive manufacturing of a variety of metallic components using deformable metal powders. In CS deposition, gas type, gas pressure, gas temperature, and powder feed rate are the four key process parameters that have been intensively studied. Spray angle, spray gun traverse speed, and standoff distance (SoD) are the other three process parameters that have been less investigated but are also important, especially when depositing on uneven substrates or building up 3D freeform structures. Herein, the effects of spray angle, traverse speed, and SoD during CS deposition have been investigated holistically on a single material system (i.e., Al2219 powders on Al2219-T6 substrate). The coatings’ mass gain, thickness, porosity, and residual stress have been characterized, and the results show that spray angle and traverse speed exercise much more effects than SoD in determining coatings’ buildup. Finite element method (FEM) modeling and computational fluid dynamic (CFD) simulation have been carried out to understand the effects of these three parameters for implementing CS as repairing and additive manufacturing using aluminum-based alloy powders.