Plasma spray-physical vapor deposition (PS-PVD) as a novel process was used to prepare feather-like columnar thermal barrier coatings (TBCs). This special microstructure shows good strain tolerance and non-line-of-sight (NLOS) deposition, giving great potential application in aero-engine. However, due to serious service environment of aero-engine, particle erosion performance is a weakness for PS-PVD 7YSZ TBCs. As a solution, an Al-modification approach was proposed in this investigation. Through in-situ reaction of Al and ZrO₂, an α-Al₂O₃ overlay can be formed on the surface of 7YSZ columnar coating. The results demonstrate that this approach can improve particle erosion resistance since hardness improvement of Al-modified TBCs. Meanwhile, as another important performance of thermal cycle, it has a better optimization with 350-cycle water-quenching, compared with the as-sprayed TBCs.