Post-harvest crop residues are an interesting raw material for the production of composite materials. However, their surface often contains waxy and siliceous substances, which can cause adhesion problems. Therefore, various surface pre-treatment methods have been developed to increase the surface tension of these particles and hence to improve adhesive adhesion. The influence of hydrothermal, chemical, plasma and enzymatic treatment was investigated. The aim of the paper is to evaluate the effect of pre-treatments of post-harvest crop residues on the nature of joint failure and adhesive dispersion on the particles. The evaluation is based on microscopic analysis of particles obtained from the rupture area after internal bonding tests. The nature of bond failure and adhesive dispersion on the particle surface is evaluated. The results show a clear influence of material pre-treatment on the failure bond of the bond and, to a large extent, correlate with the mechanical properties of composites published in previous studies. The most suitable treatment appears to be a plasma treatment at a properly adjusted intensity. Conversely, the unsuitable treatment was alkaline, which, although it increased adhesion, deteriorated the overall mechanical properties. Hydrothermal treatment could be also considered as an industrially suitable method.