This chapter introduces various extended non-destructive testing (ENDT) techniques for surface quality assessment, which are first characterized, then enhanced, and finally applied to assess the level of pre-bond contaminations intentionally applied to carbon fiber reinforced plastic (CFRP) adherends following the procedures described in the previous chapter. Based on two user cases comprising different scenarios that are characteristic of either aeronautical production or repair, the detailed tests conducted on two types of sample geometry, namely flat coupons and scarfed pilot samples with a more complex shape, form the basis for applying the advanced ENDT procedures for the monitoring of realistic and real aircraft parts, as will be described in Chap. 10.1007/978-3-319-92810-4_5. Specifically, the reported investigations were performed to assess the surface quality of first ground and then intentionally contaminated CFRP surfaces using the following ENDT tools: the aerosol wetting test (AWT), optically stimulated electron emission (OSEE), two differently implemented approaches based on electronic noses, laser-induced breakdown spectroscopy (LIBS), Fourier-transform infrared (FTIR) spectroscopy, laser-induced fluorescence (LIF), and laser vibrometry.