This preview discusses the emergent new paradigm of structural complexity engineering, featuring two recent studies on an aperiodic metal-organic framework and nanoassembly of a symmetry-breaking chiral continuum bowtie. These structurally complex materials are not ordered but also not completely random, with controlled lowered symmetry. This preview discusses the emergent new paradigm of structural complexity engineering, featuring two recent studies on an aperiodic metal-organic framework and nanoassembly of a symmetry-breaking chiral continuum bowtie. These structurally complex materials are not ordered but also not completely random, with controlled lowered symmetry.