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[Display omitted] • Arc nanosynthesis of graphite-coated magnetic core-Au satellite nanoassembly. • Tailorable nanostructure and tunable surface functionalization of FeAu@G. • Different formation mechanisms of shells over cores and satellites enable FeAu@G. • Excellent negative linearity of Cr(VI) removal time with [Au wt.%]/[Au diameter]3. • Excellent negative linearity of K values to the diameter of Au satellites. Most magnetoplasmonic nanoassemblies with tunable geometries are commonly fabricated by the wet assembly approach, which is greatly restricted by the high complexity and severe conditions. This study applied a facile one-step arc discharge to fabricate graphite-encapsulated magnetic core-gold satellite (FeAu@G) nanoassembly with tailorable morphologies (35.5–58.8 nm of magnetic cores with 4.91- 0.335 nm of shells, and 4.63–9.01 nm of Au satellites with 1–4 graphite layers of shells) and tunable surface functionalization (hydrophobization, amination). The specific formation processes of graphite shells (i.e., dissolution-reprecipitation-graphitization for shells over magnetic cores, deposition-graphitization for shells over Au satellites) is essential to generate this unique nanoassembly. An storage-dependent consuming time for the removal of Cr(VI) by aminated FeAu@G presented an excellent negative linearity with [Au wt.%]/[Au satellite diameter]3. The reusability of aminated FeAu@G could be significantly aroused by the radio-frequency plasma treatment with an enhancement of 198–894 %. Hydrophobic FeAu@G could converse nitroaromatics recycled with an excellent negative linearity of catalytic activity values to the diameter of Au satellites. This work unlocks a versatile platform to design and produce magnetoplasmonic nanoassemblies with ideal complex nanostructures and surface functionality. [ABSTRACT FROM AUTHOR]