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In movie productions, the Foley Artist is responsible for creating an overlay soundtrack that helps the movie come alive for the audience. This requires the artist to first identify the sounds that will enhance the experience for the listener thereby reinforcing the Directors's intention for a given scene. In this paper, we present AutoFoley, a fully-automated deep learning tool that can be used to synthesize a representative audio track for videos. AutoFoley can be used in the applications where there is either no corresponding audio file associated with the video or in cases where there is a need to identify critical scenarios and provide a synthesized, reinforced soundtrack. An important performance criterion of the synthesized soundtrack is to be time-synchronized with the input video, which provides for a realistic and believable portrayal of the synthesized sound. Unlike existing sound prediction and generation architectures, our algorithm is capable of precise recognition of actions as well as inter-frame relations in fast moving video clips by incorporating an interpolation technique and Temporal Relationship Networks (TRN). We employ a robust multi-scale Recurrent Neural Network (RNN) associated with a Convolutional Neural Network (CNN) for a better understanding of the intricate input-to-output associations over time. To evaluate AutoFoley, we create and introduce a large scale audio-video dataset containing a variety of sounds frequently used as Foley effects in movies. Our experiments show that the synthesized sounds are realistically portrayed with accurate temporal synchronization of the associated visual inputs. Human qualitative testing of AutoFoley show over 73% of the test subjects considered the generated soundtrack as original, which is a noteworthy improvement in cross-modal research in sound synthesis.