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Green, efficient and sustainable treatment of secondary resources such as electronic waste (e-waste) has significant strategic, economic and environmental value for the future social development, but it remains a serious task. Here, an intelligent yolk–shell-structured ion-imprinted magnetic mesoporous nanorobot (MMNR-IIP-YS) was assessed for rapid and selective gold stripping from leaching solutions from e-waste leachates and employed for water decontamination by targeting organic contaminants. MMNR-IIP-YS exhibited a competitive adsorption capacity (65.01 mg g–1) which was 2.69 times that of the non-imprinted polymer (24.16 mg g–1) at 298 K and possesses superior adsorption rate, excellent selectivity, long-term stability, and recycling ability. Interestingly, a closed-loop miniplant was established for sustainable treatment of e-waste, revealing that MMNR-IIP-YS was capable of extracting 98.51% of gold from actual waste leachates and showing efficient and stable degradation efficiency of toxic organics and dyes. These findings have the potential for application in industrial-scale treatment of e-waste and suggest an appealing strategy based on self-propelled nanorobots for future development of sustainable waste utilization systems.