Thermal　spray　coatings　are　widely　used　in　many　applications,　and　the　adhesion　effect　at　the　coating/substrate　interface　plays　an　important　role　during　the　service　life.　The　thermal　spraying　coating　and　substrate　is　primarily　combined　by　a　mechanical　seizure　effect.　In　this　work,　a　strategy　to　generate　interfacial　metallurgical　bonding　is　proposed.　Plasma　spraying　with　wire　feeding　was　adopted　to　increase　the　size　of　sprayed　particles,　and　metallurgical　bonding　was　clearly　formed　between　deposited　particles　and　the　substrate　(304　stainless-steel　and　7075　aluminum　alloy).　Interface　reaction　can　be　found　at　both　NiAl/7075　and　NiAl/304　interfaces.　Typical　Al-Al3Ni　eutectic　phase　with　higher　microhardness　was　formed　at　NiAl/7075　interface.　The　adhesive　strength　of　the　coatings　was　significantly　improved　to　82.67　+/-　3.96　MPa　and　64.45　+/-　2.84　MPa,　respectively,　for　NiAl　coating　on　304　and　7075　substrates　through　tensile　adhesion　tests　(TAT)　without　surface　roughening　pretreatment.　This　technique　shows　a　promising　aspect　of　the　application　of　thermal　spray　coatings.