In this study, based on the differences in the coordination configurations of various alkaline earth metal ions (Ca(Ⅱ) and Sr(Ⅱ)) and sodium alginate (SA), the aerogel is functionalized with controllable slit-shaped pores structure, contributing by nanosheet stacking impact of graphene oxide (GO) and montmorillonite (MMT), which is able to selectively remove plane hydrate copper ions in complex wastewater systems. Sr-G/M is endowed with denser slit-shaped pores and could achieve more efficient selective removal of Cu(Ⅱ), together with a best removal efficiency of 97.1%, proving by systematic adsorption tests. The selectivity tests show that Sr-G/M exhibits preferential adsorption for Cu(Ⅱ) with a distribution coefficient of 41.85 L g-1. Furthermore, Sr-G/M has excellent regeneration performance to be 86.4% after 8 recycles. Considering its cost-effectiveness, eco-friendliness, easy preparation and efficient selective removal performance, Sr-G/M holds great promise in selective removal of Cu(Ⅱ) from complex wastewater systems.