Interpenetrated metal-organic frameworks (MOFs) comprise two or more lattices that are mutually entangled. Interpenetration tunes the structures and pore architectures of MOFs to influence their interactions with guest molecules. Typically, the interpenetrating sublattices are identical. Hetero-interpenetrated MOFs, in contrast, have sublattices that are different to one another. While they can be produced by serendipity, to develop a deliberate strategy for making hetero-interpenetrated MOFs we employed the cubic 𝛂-MUF-9 framework as a host sublattice. 𝛂-MUF-9 is able to template the secondary growth of a second, interpenetrating, sublattice in its pores to produce hetero-interpenetrated MOFs. In certain cases, the sublattices cannot be produced via standalone reactions and are observed here for the first time. Unique functional properties are enabled by hetero-interpenetrated MOFs such as asymmetric catalysis. We grew a catalytically-active sublattice inside 𝛂-MUF-10, a chiral host. The chiral pore environment of the host imparts asymmetry on the catalytic activity of interpenetrating sublattice to give reaction products with an enantiomeric excess. This deliberate strategy for synthesizing hetero-interpenetrated MOFs opens new perspectives on framework structures and pore environments and allows unprecedented functional properties to emerge.