Function implementation and optimization in nanoscale and quantum-electronic devices become increasingly challenging with the growing complexity of the devices. Training a deep neural network with the physical device response and searching for the functionality in the digital device can ease this challenge. Many nanoscale devices require precise optimization to function. Tuning them to the desired operation regime becomes increasingly difficult and time-consuming when the number of terminals and couplings grows. Imperfections and device-to-device variations hinder optimization that uses physics-based models. Deep neural networks (DNNs) can model various complex physical phenomena but, so far, are mainly used as predictive tools. Here, we propose a generic deep-learning approach to efficiently optimize complex, multi-terminal nanoelectronic devices for desired functionality. We demonstrate our approach for realizing functionality in a disordered network of dopant atoms in silicon. We model the input-output characteristics of the device with a DNN, and subsequently optimize control parameters in the DNN model through gradient descent to realize various classification tasks. When the corresponding control settings are applied to the physical device, the resulting functionality is as predicted by the DNN model. We expect our approach to contribute to fast, in situ optimization of complex (quantum) nanoelectronic devices.