Magnetic Graphene Composites: From Rational Synthesis, Structural Design to Multifunctional Applications

Magnetic graphene composites have emerged as a frontier material platform, offering designable properties and multifunctional integration across environmental, biomedical, electromagnetic, and energy applications. Despite extensive research, a coherent knowledge framework that systematically connects synthesis, structure, property, and application remains lacking. This review addresses this gap by establishing an integrated “synthesis–structure–property–application” design paradigm. We first propose a four-tier evolutionary framework for synthesis strategies, tracing the progression from modular in-situ assembly, substrate-guided single-component in-situ formation, and synchronous in-situ formation to molecular-scale precursor co-conversion. This framework reveals the causative relationships between synthesis pathways and microstructures, and culminates in an application-oriented synthesis decision-making tool that enables rational strategy selection. Building on this synthesis foundation, we systematically analyze three core structural regulation strategies—interface engineering, defect and doping engineering, and hierarchical structure construction—demonstrating how they function as synergistic “control knobs” for tailoring composite properties. Through detailed case studies across four application domains, we quantitatively show how targeted structural design drives performance breakthroughs: enabling high-capacity and selective pollutant removal in environmental remediation; constructing intelligent theranostic platforms in biomedicine; reconciling the “thin, lightweight, broadband, and strong” paradox in electromagnetic interference (EMI) shielding; and ensuring long-cycle stability of high-capacity electrodes in energy storage. Finally, we summarize the paradigm shift from “functional combination” to “performance synergy” and outline future directions, including dynamic intelligent systems, sustainable manufacturing, and data-driven design. This review provides a systematic theoretical framework and practical roadmap for the rational design and on-demand fabrication of MGCs, marking the field’s transition from empirical exploration toward predictive, design-driven science.