This paper describes the surface characteristics of ZnO nanostructured CFRP composites in high speed microdrilling process. Two different nanostructured composites have been developed by varying the molar concentration of ZnO growth solution from 15 to 25 mM by hydrothermal method. Further, high speed microdrilling operations have been performed on those nanostructured CFRP composites along with unstructured one. Three different levels of spindle rotational speeds (25000, 37500, and 50000 rpm) and feed rates (1 µm/rev, 3 µm/rev, and 6 µm/rev) have been incorporated in the machining operation. The average surface roughness, delamination, circularity, and burr height have been measured. All those parameters have been improved significantly for nanostructured composites as compared to unstructured one. The best surface finish has been found on 15 mM ZnO nanostructured composite at 50000 rpm and 3 µm/rev feed rate with an average surface roughness of 1.88 µm. Favourable machining conditions have been achieved at elevated rotational speed and enhanced feed rate during the microdrilling operation of CFRP composites.