Block copolymers have unique associative properties that facilitate self-assembly into nanostructures that have been widely used in soft lithography, [1] templating, [2] drug delivery, [3] biomedical, [4,5] and chemical catalytic [6] applications. Of special interest is the in situ preparation of metallic or semiconducting nanoparticles in amphiphilic block copolymers. [7][8][9][10][11][12] The synthesis of nanoparticles in block copolymer micelles solves the problem of particle size control and stabilization compared to classical stabilization systems that employ surfactants [13][14][15] or microemulsions. [16,17] Nanocrystal-based organic memories [18][19][20][21] are attracting widespread interest owing to their simple structure and the prospect of creating 2D/3D stacks of these memory cells for increased bit densities. Recent reviews [20,22,28] summarize the literature for these nanoparticle-based organic memories comprehensively, and have identified the main operating mechanisms to be one of the following: (i) an electricfield-induced charge transfer between the nanoparticles and the surrounding conjugated compounds, [19,22] (ii) filamentary conduction, [23,24] (iii) charge trapping-detrapping, [25,26] and (iv) space-charge field inhibition of injection in the nanoparticles through a high-voltage pulse. [20,27] Besides the widely used two-terminal bistable organic memory devices, an alternative memory architecture that can be adopted is based on an organic thin-film transistor (OTFT) with a non-volatile floating gate memory [29] which allows a direct integration of the memory element with the transistor for integrated circuit applications. The ability to have a one-step fabrication process to generate arrays of metallic nanoparticles using solutionprocessing methods makes this approach amenable to potential implementations in the nanoparticle-based organic memory devices mentioned above. This is in contrast to past designs of organic memory devices, which involved the use of multistep approaches of presynthesizing nanoparticles followed by surface modification to prevent agglomeration prior to embedding them in multiple functional layers through solution processing or physical vapor deposition. Furthermore, this solution-processing approach is especially suitable for low-cost, large-area processing on flexible substrates, which may be considered to be the cornerstone of organic electronics applications. We demonstrate herein, for the first time, a polymeric memory that comprises an in situ synthesis strategy of gold nanoparticles in polystyrene-block-poly(4-vinylpyridine) (PS-b-P4VP). This system serves as a prototype for a generic memory device using nanoparticles as floating gate charge storage centers and, in particular, for integration into OTFT-based circuits. The block copolymer micelles turn out to be an excellent model system that is simple, forms a self-assembled ordered nanostructure, and provides optimum control over nanoparticle size formation and isolation. The response of the memory device is c...