Methods are provided for mechanically chopping nanotubes and other nanoscale fibrous materials. The method includes forming a macroscale article which include the nanoscale fibers, and then mechanically cutting the macroscale article into a finely divided form. In one embodiment, these steps are repeated. The nanoscale fibers may be carbon nanotubes, which optionally are aligned in the macroscale article. The macroscale article may be in the form of or include one or more buckypapers. In one embodiment, the macroscale article further includes a solid matrix material in which the nanoscale fibers are contained or dispersed. The forming step can include making a suspension of nanoscale fibers dispersed in a liquid medium and then solidifying the liquid medium to form the macroscale article. After the mechanical cutting step, the medium can be dissolved or melted to enable separation of the chopped nanoscale fibers from the medium.