Textiles have always been one of the essential materials for people and have a great variety of uses such as in clothing, agriculture, medical, automotive and aerospace applications. The sort of properties needed for any type of fabric basically depend on the structure of the fibre surface. Of many geometric attributes that can be used to describe the surface appearance of a fibre, yarn, or fabric sample, one of the more common is lustre. Mohair and wool fibre surface structure have been studied using optical microscopy and Atomic Force Microscopy (AFM). Optical microscopy was also used to take fibre diameter measurements. Another technique, goniophotometry, was used to make quantitative lustre measurements of mohair and wool fibres. The surface structure of mohair has got a faint pattern of scales where the scales are generally unpronounced or flat and relatively long. Wool has got a scaly surface structure where the scales overlap leading to interlocking of fibres. The scale configuration on the surface of mohair and wool fibres also differs. A qualitative connection between fibre lustre and the fibre surface structure was found. Because of its smooth surface relative to that of wool, mohair reflects a greater amount of incident light specularly whereas wool reflects most of the incident light diffusely. In general, mohair fibres have a higher lustre than wool due to its less prominent cuticle structure found on its surface. Furthermore, mohair fibres with the smallest diameters give an even higher lustre.