A layered double hydroxide (LDH) calcined-framework adsorbent was investigated for the rapid removal of heavy metal cations from plating wastewater. Li–Al–CO3LDH was synthesized on an aluminum lathe waste frame surface to prepare the sorbent. The calcination treatment modified the LDH surface properties, such as the hydrophilicity and the surface pH. The change in surface functional groups and the leaching of lithium ions affected the surface properties and the adsorption capacity of the heavy metal cations. A zeta potential analysis confirmed that the 400 °C calcination changed the LDH surface from positively charged (+10 mV) to negatively charged (−17 mV). This negatively charged surface contributed to the sorbent instantly bonding with heavy metal cations in large quantities, as occurs during contact with wastewater. The adsorption isotherms could be fitted using the Freundlich model. The pseudo-second-order model and the rate-controlled liquid-film diffusion model successfully simulated the adsorption kinetics, suggesting that the critical adsorption step was a heterogeneous surface reaction. This study also confirmed that the recovered nickel and/or copper species could be converted into supported metal nanoparticles with a high-temperature hydrogen reduction treatment, which could be reused as catalysts.