The advances of Deep Learning (DL) achieved recently have successfully demonstrated its great potential of surpassing or close to human-level performance across multiple domains. Consequently, there exists a rising demand to deploy state-of-the-art DL algorithms, e.g., Deep Neural Networks (DNN), in real-world applications to release labors from repetitive work. On the one hand, the impressive performance achieved by the DNN normally accompanies with the drawbacks of intensive memory and power usage due to enormous model size and high computation workload, which significantly hampers their deployment on the resource-limited cyber-physical systems or edge devices. Thus, the urgent demand for enhancing the inference efficiency of DNN has also great research interests across various communities. On the other hand, scientists and engineers still have insufficient knowledge about the principles of DNN which makes it mostly be treated as a black-box. Under such circumstance, DNN is like "the sword of Damocles" where its security or fault-tolerance capability is an essential concern which cannot be circumvented.

Motivated by the aforementioned concerns, this dissertation comprehensively investigates the emerging efficiency and security issues of DNNs, from both software and hardware design perspectives. From the efficiency perspective, as the foundation technique for efficient inference of target DNN, the model compression via quantization is elaborated. In order to maximize the inference performance boost, the deployment of quantized DNN on the revolutionary Computing-in-Memory based neural accelerator is presented in a cross-layer (device/circuit/system) fashion. From the security perspective, the well known adversarial attack is investigated spanning from its original input attack form (aka. Adversarial example generation) to its parameter attack variant.