plasmonic chirality has the characteristics of strong signal, wide spectral window, and dynamic controllability and holds huge promises in a wide range of applications, [2] such as metamaterials, [3] ultrasensitive detection, [4] enantioselective separation, [5] disease diagnosis (such as Parkinsons [6]), and chiral catalysis. [7] The rapid development of chiroplasmonics not only advances the nanoplasmonics itself but also renovates the old research field of molecular chirality. Apart from preparing discrete plasmonic chiral nanostructures, [3,8] chiral assemblies of plasmonic nanoparticles have attracted more attention owing to easy fabrication and feasible dynamic modulation. [9] Often, the most straightforward and simple way is to organize non-chiral plasmonic NPs using various chiral templates, [10] such as DNA, [4a,11] chiral fibers, and so on [6,12] into a chiral arrangement along the templates. In contrast, it's more difficult and challenging to drive a non-chiral (racemic) assembly into a chiral one (high enantiomeric excess) from the viewpoint of using chiral forces. [13] Previously, we tackled this issue by adsorbing small chiral molecules on non-chiral side-by-side (SS) assemblies of gold nanorods (AuNRs). [14] The chiral forces provided by the adsorbed chiral thiols can convert the non-chiral assemblies into chiral ones. Furthermore, by reducing the assemblies to AuNR dimers, the chirality can be manipulated by circularly polarized lights. [13a] More intriguing, when such chiral assemblies of AuNRs are annealed at elevated temperatures, the plasmonic circular dichroism (PCD) responses can be further amplified with an anisotropic g factor of reaching ≈0.065. [14c] Considering the easy implementation of this treatment, we wonder whether this phenomenon is universal and can be utilized as a general way to modulate chiroptical responses driven by small chiral molecules. From the viewpoints of same crystal structure with similar lattice constants but stronger plasmonic responses, Ag is our first choice. [15] Herein, an Ag shell was formed on the AuNR to expose Ag. The obtained AuNR@Ag was used as assembly unit to form side-by-side oligomers. AuNR@Ag oligomers are used to research PCD temperature amplification effect. However, the maximal annealing temperature of showing PCD amplification Achieving huge chiroptical responses is one of the driving forces for the applications of plasmonic metamaterials. Heat-assisted symmetry breaking can amplify plasmonic circular dichroism (PCD) signals in Au nanorod (AuNR) oligomers; however, the PCD responses disappear on Ag-exposed surface (AuNR@Ag core-shell nanorods) at high temperature. Thus, the inherent reason of different chiral response between Au-and Ag-surface nanorods oligomers is explored, and the chiral mechanism is further cognized. The enhanced mobility of surface Ag atoms at elevated temperatures leads to the damage of cysteine chiral networks on Ag surface. It therefore causes great reduction of chiral drive forces, thus restricting the PCD temperature am...