Layered double hydroxidesLayered double hydroxides (LDH) possess a distinctive feature known as theStructural memory effect “structural memory effectMemory effect” enabling them to reconstruct their layered structure destroyed by calcination at temperatures below 600 °C. This characteristic empowers the regenerated LDH structures as promising candidates for a variety of applications. While most studies have concentrated on the structural regeneration of LDH and their derived layered double oxides (LDO) as separate phases, the primary objective of this work is to explore how cycles of calcination followed by structural reconstruction of certain transition metal-based LDH can produce entangled LDH–LDO composites. This tunable calcination-reconstructionCalcination-reconstruction approach can be valorized as a novel strategy for designing LDH–LDO nanohybrids that combine the functional properties of both structural units. Our findings revealed that repeated cycles of calcination and reconstruction in ZnAlLDH, NiAlLDH, and ZnFeLDH yield hybrid structures identified as ZnAlLDH–ZnO, NiAlLDH–NiO, and ZnFeLDH–ZnO, respectively. Conversely, under the experimental conditions applied in this study, NiFeLDH did not show structural recovery. Furthermore, we found that the extent to which the regenerated LDH contributes to the composite structure is significantly influenced by the number of calcination-reconstructionCalcination-reconstruction cycles. These hybrids exhibit potential for enhanced performance in catalysisCatalysis and open new avenues for advanced technological applications.