WFeNi(Ti) and MoFeNi(Ti) alloy layers were fabricated onto Ti surfaces from W, Mo, and Ni targets through ball collisions initiated by a mechanically vibrated vial. The as-fabricated alloy structures could be represented as a heterogeneous multi-modal nanocrystalline structure with elemental flakes embedded within a matrix composed of nanocrystalline grains encapsulated within an amorphous phase. The deformation-induced chemical interactions between dissimilar atoms in the WFeNi(Ti) and MoFeNi(Ti) systems affected the structural formation of the alloy layers. Fe atoms in the WFeNi(Ti) alloy system tended to react with Ni, forming fcc (Fe,Ni) phase, while W atoms dissolved into the fcc (Fe,Ni) lattice. In the MoFeNi(Ti) alloy system, Fe tended to react with Mo over Ni, resulting in the formation of a bcc Fe(NiMo) solid solution. The Ti particles absorbed oxygen atoms. Chemical interactions between Ti and oxygen atoms made the Ti and oxygen components passive with regard to other present metallic elements.