The analysis of explosives attracts recent research efforts due to homeland security needs and the broad demand for the clearance of minefields. While numerous studies have addressed the development of sensing platforms for nitroaromatic explosives, and specifically trinitrotoluene (TNT), the detection of more hazardous explosives, such as hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) or pentaerythritol tetranitrate (PETN), is less developed and needs further efforts, particularly the improvement of the sensitivities associated with the analyses of these substrates.[1,2] Different optical, electrochemical, or microgravimetric sensors or biosensors for TNT were reported. Fluorescent organic polymers, which are quenched by nitroaromatic explosives, [3,4] luminescent polysilole nanoparticles (NPs), [5,6] or fluorescent silicon NPs quenched by nitroaromatic vapors enabled the development of optical sensors. The electrochemical activity of the nitro groups of TNT provided the basis for developing voltammetric sensors for this explosive, [7,8] and recently, a composite of Au NPs linked to electrodes enabled a sensitive electrochemical detection of TNT.[9] Also, different sensing matrices, such as cyclodextrin polymers, [10] carbowax, [11] or silicon polymers, [12] were used for TNT analysis by surface acoustic wave devices, and the aggregation of functionalized Au NPs in the presence of TNT was used to develop an optical sensor for the explosive.[13] Similarly, antibody-based optical [14][15][16] or microgravimetric quartz-crystal-microbalance [17] biosensors for TNT were developed. Different optical [18,19] or voltammetric [20] sensors for RDX were also reported. These included the fluorescence detection of RDX with an acridinium dye, [18] or the application of NADH-functionalized quantum dots.[21] Also, a competitive fluorescence immunoassay for the detection of RDX was reported.[22] The sensitivities accomplished by these methods are, however, unsatisfactory for analyzing trace amounts of the RDX explosive.Surface plasmon resonance (SPR) is a versatile method for probing changes in the refractive index occurring on thin metal films as a result of recognition events or chemical reactions. [23,24] Numerous SPR sensors and biosensors were developed, [25][26][27] and metal NPs were implemented to enhance the SPR response and to amplify SPR-based sensors. [28,29] The electronic coupling between the localized plasmon of the metallic NPs (e.g., Au NPs) and the surface plasmon wave enhances the SPR response and, thus, the labeling of recognition complexes with metallic NPs amplifies the sensing events. Different biosensing processes, such as DNA hybridization, [30] formation of immunocomplexes, [31] and the probing of biocatalytic transformations, [32] used Au NPs as labels for amplified SPR analyses. Recently, composites of bisaniline-crosslinked Au NPs were electropolymerized on Au electrodes, and the resulting matrices were used for the ultrasensitive SPR detection of TNT.[33] The formation of p-donor-acceptor complexes ...