decade, many approaches for synthesizing multifunctional NPs with combined properties have been developed, such as heterogeneous crystal growth, [3][4][5] coassembly of different building blocks, [6,7] and the template-based method involving chemical and/or physical binding. [8,9] In particular, the template-based method is advantageous for utilizing the size-and shape-dependent properties of individual NPs, [8][9][10] new properties resulting from inter-particle coupling, [8,10,11] and independently additional modification of different NPs and the template. [11,12] Among the various multifunctional NPs, magnetic-plasmonic (MP) NPs are regarded as emerging materials that are suitable for a broad range of applications, such as catalysis, [12,13] detection, [14,15] optical devices, [9,16] and therapy. [17][18][19] In particular, MP NPs simultaneously exhibiting magnetic and surface-enhanced Raman scattering (SERS) activities have been researched due to their synergistic properties in biomedical applications. [20][21][22][23][24] In detail, non-destructive and sensitive analysis of the SERS technique and separating ability based on the magnetic properties could provide convenient and significant tools in sensing of target molecules or cells. [20][21][22][23][24][25] However, it is difficult to satisfy the designing criteria for high performances in bio-applications: low remanence for preventing particle aggregation, maximized magnetic Magnetic-plasmonic nanoparticles have received considerable attention for widespread applications. These nanoparticles (NPs) exhibiting surfaceenhanced Raman scattering (SERS) activities are developed due to their potential in bio-sensing applicable in non-destructive and sensitive analysis with target-specific separation. However, it is challenging to synthesize these NPs that simultaneously exhibit low remanence, maximized magnetic content, plasmonic coverage with abundant hotspots, and structural uniformity. Here, a method that involves the conjugation of a magnetic template with gold seeds via chemical binding and seed-mediated growth is proposed, with the objective of obtaining plasmonic nanostructures with abundant hotspots on a magnetic template. To obtain a clean surface for directly functionalizing ligands and enhancing the Raman intensity, an additional growth step of gold (Au) and/or silver (Ag) atoms is proposed after modifying the Raman molecules on the as-prepared magnetic-plasmonic nanoparticles. Importantly, one-sided silver growth occurred in an environment where gold facets are blocked by Raman molecules; otherwise, the gold growth is layer-by-layer. Moreover, simultaneous reduction by gold and silver ions allowed for the formation of a uniform bimetallic layer. The enhancement factor of the nanoparticles with a bimetallic layer is approximately 10 7 . The SERS probes functionalized cyclic peptides are employed for targeted cancer-cell imaging and separation.