The design of new chiral materials usually requires stereoselective organic synthesis to create molecules with chiral centers. Less commonly, achiral molecules can self-assemble into chiral materials, despite the absence of intrinsic molecular chirality. Here, we demonstrate the assembly of high-symmetry molecules into a chiral van der Waals structure by synthesizing crystals of C-60(SnI4)(2) from icosahedral buckminsterfullerene (C-60) and tetrahedral SnI4 molecules through spontaneous self-assembly. The SnI4 tetrahedra template the Sn atoms into a chiral cubic three-connected net of the SrSi2 type. Our results represent the remarkable emergence of a self-assembled chiral material from two of the most highly symmetric molecules, demonstrating that almost any molecular, nanocrystalline, or engineered precursor can be considered when designing chiral assemblies.