A mechanism of inelastic deformation of freestanding plasma-sprayed thermal barrier coatings (TBCs) has been clarified. Cantilever-type bending tests are carried out inside SEM chamber in order to obtain a stress-strain curve of the freestanding ceramic coating peeled from the TBC coated sample by an electrochemical treatment and reveal the associated microstructure changes such as splats or splat boundaries. The bending test result indicated that the coating deforms with a nonlinear behavior under monotonic loading. In-flight particle velocity in the spraying parameter affected the stress-strain curve significantly. In-situ SEM observation during bending loading revealed that sliding at the boundaries between splats plays an important role in an inelastic deformation.