The development of nanoâmanufacture technology in the twentyâfirst century has paved the way for artificial nanostructure constructions like manâmade superlattices, providing historical breakthroughs in thermal physics and thermoelectrics by the modulation of phonons. Still, highâperformance thermal insulators haven't come into operation due to the arduousness, costing and unscalability of artificiality. Herein, intentional engineering on a soâcalled ânatural superlatticeâ with alternating PbSeâ and Bi2Se3âlayer crystal structure is brought forth to recreate the mechanism of artificial superlattices and boost phonon localization. The thermal conductivity notably shows a directionâspecific reduction, leading to minimum approaching and enhanced anisotropy. The modification of the natural framework and its effects have been supported by various transport and structure studies. This work sets a generalizable example for natural layered material engineering that bridges between the inflexible, changeless but selfâassembled natural layered compounds, and the highly efficient, delicately tailored but unscalable artificial superlattice complexes. The methodology promises new horizons for practicable thermal management.