The metallurgical bonding of cold spraying is investigated from the perspective of plastic deformation. The individual Al particle was deposited on the surface of Ni substrate by low-pressure cold spraying technology. Direct observation of the Al/Ni interface from the cross-sectional morphology shows that metallurgical bonding occurs only at the partial Al/Ni interface. The finite element simulation considering the presence of oxide layer confirms that the metallurgical bonding is located in front of the maximum plastic deformation area. In the maximum plastic deformation area, the relative displacement between Al particle and Ni substrate exists from the beginning of contact to the end of deposition, which makes the metallurgical bonding discontinuous and gradually disappear.