units (GPUs) and >1000 central processing units (CPUs) for some of the highest performance demonstrations. [4] In order to approach the massively parallel and energy efficient operation of the brain (â25 W), [7] neuromorphic computing architectures have been proposed which utilize physical processes in materials to emulate synaptic behavior. [8][9][10] Among these, resistive memory (memristive) devices [11,12] have gained traction as a highly suitable option, offering projected efficiency gains of up to 10 6 over von Neumann architectures when implementing ANN algorithms. [13,14] Efficiency gains originate from parallel computation and scale with array size (N) [15] : an N Ă N sized neuromorphic array can simultaneously perform N 2 operations using Ohm's and Kirchoff's laws (multiply and accumulate, respectively), whereas GPUs can perform only N operations simultaneously.Nonvolatile memristive devices such as phase change memory (PCM) and resistive random-access memory (ReRAM) have been proposed for use as nonvolatile artificial synapses due to their ability to tune the resistance state by applied voltage pulses. [16][17][18] By arranging these devices in a crossbar array architecture, vector-matrix multiplication (VMM) can be performed in an analog fashion where the input vector is represented by voltages, the operator matrix is represented by the conductance of each memristive element, and the output vector is represented by currents. These crossbar arrays have recently been implemented in a dot-product engine which uses VMM operations to classify handwritten digits with â90% accuracy. [19] However, this demonstration requires a timeconsuming feedback programming scheme which reduces the parallelism of the write operation to the array and ultimately its overall efficiency.Recently, electrochemical nonvolatile redox memory (NVRM) devices [20,21] have emerged as an ideal candidate for neuromorphic arrays as they decouple read and write operations, thereby allowing for low-energy programming and accurately tunable conductance states while potentially avoiding the time-voltage dilemma. [22,23] Furthermore, organic materials are an attractive alternative to conventional resistive memory due to their linearly tunable conductance, [22] biocompatibility, [24] and unique switching mechanisms which significantly differ from their inorganic counterparts. [25][26][27][28][29][30] In particular, there has been interest in mixed ionic-electronic conductors, Recent breakthroughs in artificial neural networks (ANNs) have spurred interest in efficient computational paradigms where the energy and time costs for training and inference are reduced. One promising contender for efficient ANN implementation is crossbar arrays of resistive memory elements that emulate the synaptic strength between neurons within the ANN. Organic nonvolatile redox memory has recently been demonstrated as a promising device for neuromorphic computing, offering a continuous range of linearly programmable resistance states and tunable electronic and elect...