To enable the determination of detailed structures of nanomaterials, we extend the theory of low-energy electron diffraction ͑LEED͒ to become more efficient for complex and disordered systems. Our new cluster approach speeds up the computation to scale as n log n, rather than the current n 3 or n 2 , with n the number of atoms, for example, making nanostructures accessible. Experimental methods to measure LEED data already exist or have been proposed. Potential application to ordered nanoparticles are illustrated here for C 60 molecules adsorbed on a Cu͑111͒ surface, with and without coadsorbed metal atoms, as well as for adsorbed carbon nanotubes. These demonstrate sensitivity to important structural features such as size and deformation of the nanostructures.