Deep convolutional neural networks (ConvNets), which are at the heart of many new emerging applications, achieve remarkable performance in audio and visual recognition tasks. Unfortunately, achieving accuracy often implies significant computational costs, limiting deployability. In modern ConvNets it is typical for the convolution layers to consume the vast majority of computational resources during inference. This has made the acceleration of these layers an important research area in academia and industry. In this paper, we examine the effects of co-optimizing the internal structures of the convolutional layers and underlying implementation of fundamental convolution operation. We demonstrate that a combination of these methods can have a big impact on the overall speedup of a ConvNet, achieving a ten-fold increase over baseline. We also introduce a new class of fast one-dimensional (1D) convolutions for ConvNets using the Toom-Cook algorithm. We show that our proposed scheme is mathematically well-grounded, robust, and does not require any time-consuming retraining, while still achieving speedups solely from convolutional layers with no loss in baseline accuracy.