A wide range of biomineralization1 and templating2,3 methods exist for organizing inorganic materials at a wide range of length-scales. Here, we show that crystallographic control of the inorganic nanostructures is possible using synthetic biomolecular templates comprised of anionic DNA and cationic membranes,4 which self-assemble into a multilamellar structure where a periodic one-dimensional (1D) lattice of parallel DNA chains is confined between stacked two-dimensional (2D) lipid sheets. We have organized Cd2+ ions within the interhelical pores between DNA strands and subsequently reacted them with H2S to form CdS nanorods of controllable widths and crystallographic orientation. The strong electrostatic interactions align the templated C...